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Recently, fluorescent sensors have gained considerable attention due to their high sensitivity, low cost and noninvasiveness. Among the different materials that can be used for this purpose, carbon dots (CDs) represent valuable candidates for applications in sensing. These, indeed, are easily synthesized, show high quantum yield and are highly biocompatible. However, it was pointed out that the photoluminescence properties of these nanomaterials are strictly dependent on the synthetic and purification methods adopted. The presence of halloysite nanotubes (HNTs), a natural, low cost and biocompatible clay mineral, has been found to be efficient in obtaining small and highly monodispersed CDs without long and tedious purification techniques. Herein, we report the comparison of synthetic pathways for obtaining halloysite-N-doped CDs (HNTs-NCDs) that could be used in biological sensing. One was based on the synthesis of N-doped CDs by a bottom-up approach on HNTs’ surface by a MW pyrolysis process; the other one was based on the post-modification of pristine N-doped CDs with halloysite derivatives. The evaluation of the best synthetic route was performed by different physico-chemical techniques. It was found that the bottom-up approach led to the formation of N-doped CDs with different functional groups onto the HNTs’ surface. This evidence was also translated in the different fluorescence quantum yields and the existence of several functional groups in the obtained materials was investigated by potentiometric titrations. Furthermore, the ability of the synthesized nanomaterials as sensors for Fe3+ ions detection was assessed by spectroscopic measurements, and the cellular uptake was verified by confocal/fluorescence microscopies as well. © 2024 by the authors.

The development of fluorescent materials that can act as sensors for the determination of metal ions in biological fluids is important since they show, among others, high sensitivity and specificity. However, most of the molecules that are used for these purposes possess a very low solubility in aqueous media, and, thus, it is necessary to adopt some derivation strategies. Clay minerals, for example, hectorite, as natural materials, are biocompatible and available in large amounts at a very low cost that have been extensively used as carrier systems for the delivery of different hydrophobic species. In the present work, we report the synthesis and characterization of a hectorite/phenanthroline nanomaterial as a potential fluorescent sensor for Zn ion detection in water. The interaction of phenanthroline with the Ht interlaminar space was thoroughly investigated, via both theoretical and experimental studies (i.e., thermogravimetry, FT-IR, UV-vis and fluorescence spectroscopies and XRD measurements), while its morphology was imaged by scanning electron microscopy. Afterwards, the possibility to use it as sensor for the detection of Zn2+ ions, in comparison to other metal ions, was investigated through fluorescent measurements, and the stability of the solid Ht/Phe/Zn complex was assessed by different experimental and theoretical measurements.

Recently, fluorescent sensors have gained considerable attention due to their high sensitivity, low cost and noninvasiveness. Among the different materials that can be used for this purpose, carbon dots (CDs) represent valuable candidates for applications in sensing. These, indeed, are easily synthesized, show high quantum yield and are highly biocompatible. However, it was pointed out that the photoluminescence properties of these nanomaterials are strictly dependent on the synthetic and purification methods adopted. The presence of halloysite nanotubes (HNTs), a natural, low cost and biocompatible clay mineral, has been found to be efficient in obtaining small and highly monodispersed CDs without long and tedious purification techniques. Herein, we report the comparison of synthetic pathways for obtaining halloysite-N-doped CDs (HNTs-NCDs) that could be used in biological sensing. One was based on the synthesis of N-doped CDs by a bottom-up approach on HNTs’ surface by a MW pyrolysis process; the other one was based on the post-modification of pristine N-doped CDs with halloysite derivatives. The evaluation of the best synthetic route was performed by different physico-chemical techniques. It was found that the bottom-up approach led to the formation of N-doped CDs with different functional groups onto the HNTs’ surface. This evidence was also translated in the different fluorescence quantum yields and the existence of several functional groups in the obtained materials was investigated by potentiometric titrations. Furthermore, the ability of the synthesized nanomaterials as sensors for Fe3+ ions detection was assessed by spectroscopic measurements, and the cellular uptake was verified by confocal/fluorescence microscopies as well.

Three-dimensional (3D) printing technology has grown exponentially in pharmaceutical field allowing the development of customized formulations designed ad hoc for the patient. This technology is constantly evolving allowing the exploitation of natural and new sustainable materials suitable for 3D printing[1]. Fused deposition modeling (FDM) is the most widely used 3D printing technique. The objective is to develop flexible, homogeneous and printable corn starch filaments suitable for FDM. With this idea, they were prepared starch-based thermoplastic (TPS) filaments consisting of: 70% w/w corn starch and 30 % w/w glycerol (Gly) as plasticizer. Clays, citric acid (CA), magnesium stearate (MgSt) were added as reinforcing agents to improve the extrusion process, thermal and mechanical properties of the filament formulation. In addition, swelling capacity of the different TPS filaments was studied. The use of the cationic clays halloysite (HAL) and montmorillonite (MMT), at 2 parts per hundred parts (phr)[2] showed that HAL did not improve TPS control filament brittleness while MMT promotes a slight decrease of brittleness higher homogeneity. However, difficulties in the extrusion process were observed. A further modification consisted in the introduction of CA, added to 3 phr of TPS, and MgSt to 2 phr of TPS. CA produces a change in the polymeric interaction, decreasing the fragility. This is mainly attributed to the acidity of CA that promotes the fragmentation and dissolution of the starch granules. Additionally, CA and Gly are responsible for the rupture of inter and intramolecular hydrogen bonds, plasticizing the starch under shear and temperature conditions[3,4]. The result is a homogeneous and less fragile filament. MgSt was added to improve the filament flowability during the extrusion process[5] . The filaments were produced by hot melt extrusion (HME) at 134, 140 and 145 °C. Different filament formulations showed modified physical and chemical properties. The f

Hypothesis: Development of nanocomposite coating with antibiofilm properties is of fundamental importance to efficient fight biofilm formation preventing infections in biomedical area. In this context, halloysite nanotubes (HNTs), biocompatible and low-cost clay mineral, have been efficiently used as filler for different polymeric matrices affording several nanocomposites with appealing antimicrobial properties. The modification of HNTs surfaces represents a valuable strategy to improve the utilization of the clay for biological purposes. Experiments. Herein, the covalent modification of the HNTs lumen with properly designed dopamine derivatives with different perfluoroalkyl chain length is reported. The obtained nanomaterials are thoroughly characterized by several techniques. As proof of concept the antibiofilm properties on E. coli strain of the nanomaterials are assayed as well. Finally, the HNTs fillers were introduced into a polydopamine matrix allowing for the preparation of functional coatings, resistant to formation of microbial biofilms. Findings: All characterization methods proved the selectivity of the modification and the increased hydrophobicity of the lumen. In particular Al solid state nuclear magnetic resonance (NMR) spectra showed a upfield shift of the Al signal. Studies on the antibiofilm properties highlighted different activities according to the length of perfluoroalkyl chains of organic molecules as proved by F solid state NMR spectra. The synthetized materials were promising for future application as coatings on medical implants.

The invention relates to a method for preparing a nano-structured material of a silicate having a laminar, fibrilar or tubular structure with praziquantel, a compound with antiparasitic activity. Other aspects of the invention relate to the material obtained using the preparation method and to the use of same to eliminate parasites, both in compositions for treating parasitic diseases, particularly schistosomiasis, and in ventilation systems or water pipelines.

Vascular stents (VS) have revolutionized the treatment of cardiovascular diseases, as evidenced by the fact that the implantation of VS in coronary artery disease (CAD) patients has become a routine, easily approachable surgical intervention for the treatment of stenosed blood vessels. Despite the evolution of VS throughout the years, more efficient approaches are still required to address the medical and scientific challenges, especially when it comes to peripheral artery disease (PAD). In this regard, three-dimensional (3D) printing is envisaged as a promising alternative to upgrade VS by optimizing the shape, dimensions and stent backbone (crucial for optimal mechanical properties), making them customizable for each patient and each stenosed lesion. Moreover, the combination of 3D printing with other methods could also upgrade the final device. This review focuses on the most recent studies using 3D printing techniques to produce VS, both by itself and in combination with other techniques. The final aim is to provide an overview of the possibilities and limitations of 3D printing in the manufacturing of VS. Furthermore, the current situation of CAD and PAD pathologies is also addressed, thus highlighting the main weaknesses of the already existing VS and identifying research gaps, possible market niches and future directions.

Drug delivery systems impacted significantly biomedical research, and the number of nano- and micro-formulations recently approved for clinical trials or marketed increased. Raw materials-based drug delivery systems have currently organic and inorganic origin, and calcium carbonate particles demonstrated several potentialities in biomedical applications and controlled drug delivery as well as they are safe and biocompatible. The aim of this study was the synthesis of calcium carbonate particles to improve the dissolution rate of praziquantel, a poorly water-soluble drug which is the gold standard for the treatment of parasite infections. Calcium carbonate particles were obtained using a synthetic carbon-based approach. Physicochemical properties of calcium carbonate particles, with or without praziquantel, were carried out by using scanning electron microscopy, Fourier transformed infrared spectroscopy, X-ray powder diffraction, thermal gravimetry and differential scanning calorimetry analysis. The solid-state characterization of calcium carbonate particles demonstrated that calcite crystals are synthesized, and these crystals interact specifically with praziquantel. The release profiles of praziquantel from calcium carbonate particles were further studied using United States Pharmacopeia dissolution test and the amount of drug released was quantified by using high performance liquid chromatography. Calcium carbonate particles increased the dissolution rate of praziquantel, which is higher than pure crystalline drug. Resulting data may suggest a potential application of these inorganic particles for oral and controlled release of praziquantel and their potential use as novel therapy for human helminthes infections.

The development of systems able to deliver genetic material into a target site is a challenge for modern medicine. Single-stranded peptide nucleic acids have attracted attention as promising therapeutic molecules for diagnostic and gene therapy. However, their poor cell membrane permeability represents a drawback for biomedical applications. Halloysite nanotubes (HNTs) are emerging materials in drug delivery applications both for their ability to penetrate cell membranes and for enhancing the solubility of drugs in biological media. Herein, we report the first example of the use of a nanocarrier based on halloysite labelled with fluorescent switchable halochromic oxazine molecules, to deliver a single-stranded peptide nucleic acids tetramer (PNA) into living cells. The PNA is covalently attached to halloysite (HNTs-PNA), whereas the fluorescent probe supramolecularly interacts with HNTs. The ability of the nanomaterial to bind complementary single-stranded DNA was assessed by resonance light scattering measurements. Finally, studies of cellular uptake were carried out by confocal laser scanning microscopy on normal and tumoral cell lines. This work highlights the usefulness of the covalent approach to generate HNTs-PNA nanomaterials for the potential targeting of future specific nucleic acids in living cells, which could open the doorway to novel possibilities for theranostic and gene therapy applications.

Melatonin is a hormone used for treating several disorders. However, its oral administration is problematic due to the variable absorption and extensive first-pass metabolism. The topical application of this drug does not present these disadvantages and can be used for therapeutic and skin protection purposes. The adsorption and release of melatonin in the montmorillonite clay were investigated experimentally and theoretically. The drug-clay interaction products were prepared and characterized, showing a modified and improved release of melatonin. The crystal structure and spectroscopic properties of the crystal of melatonin and melatonin-water-mineral materials were studied by molecular modeling, finding that the adsorption of this drug is energetically favourable, and the results were consistent with the experimental data. Ab initio molecular dynamics simulations with the metadynamics methodology showed the release of melatonin from the confined interlayer nanospace of montmorillonite to the liquid bulk water with a 20 kcal/mol free energy barrier.

The goal of this work is the design and the development of scaffolds based on maltodextrin (MD) to recover chronic lesions. MD was mixed with arginine/lysine/polylysine and the electrospinning was successfully used to prepare scaffolds with uniform and continuous nanofibers having regular shape and smooth surface. A thermal treatment was applied to obtain insoluble scaffolds in aqueous environment, taking the advantage of amino acids-polysaccharide conjugates formed via Maillard-type reaction. The morphological analysis showed that the scaffolds had nanofibrous structures, and that the cross-linking by heating did not significantly change the nanofibers' dimensions and did not alter the system stability. Moreover, the heating process caused a reduction of free amino group and proportionally increased scaffold cross-linking degree. The scaffolds were elastic and resistant to break, and possessed negative zeta potential in physiological fluids. These were characterized by direct antioxidant properties and Fe chelation capability (indirect antioxidant properties). Moreover, the scaffolds were cytocompatible towards fibroblasts and monocytes-derived macrophages, and did not show any significant pro-inflammatory activity. Finally, those proved to accelerate the recovery of the burn/excisional wounds. Considering all the features, MD-poly/amino acids scaffolds could be considered as promising medical devices for the treatment of chronic wounds.

Nanocomposites formed by clay and lipid carriers (NLCs) show a high potential for providing controlled release and specific delivery of bioactive molecules and have recently gained attention in the pharmaceutical sector due to their ability to transport hydrophilic and hydrophobic drugs. Recent studies have recognized the biological activity of the oil of Bixa orellana L. (AO) with regards to its healing, antioxidant, antibacterial, and anti-leishmanial properties. Therefore, the purpose of this study is the preparation and characterization of hybrid systems based on lipid nanocarriers and laponite for the delivery of AO. NLCs were prepared by the fusion-emulsification method, using cetyl palmitate (CP) or myristyl myristate (MM), AO, and Poloxamer 188. The morphology, hydrodynamic diameters, zeta potential (ZP), polydispersity index (PDI), thermal analysis, X-ray diffraction analysis (XRD), viscosity behavior, and cytotoxicity testing of the hybrid systems were performed. The thermal study and X-ray diffraction analyses (XRD) revealed polymorphic structural changes compatible with the amorphization of the material. Rheological assays highlighted a typical pseudoplastic behavior in all systems (MM and CP with LAP). The hybrid systems’ morphology, size diameters, and PDIs were similar, preset spherical and monodisperse structures (≈200 nm; <0.3), without significant change up to sixty days. The ZP values differed from each other, becoming higher with increasing AO concentration. XEDS spectra and elemental X-ray maps show peaks of lipids (organic components, C and O) and inorganic components O, Mg, and Si. All samples showed cell viability above 60%. The results indicated a stable, biocompatible hybrid system that can be an alternative for topical application.

This work developed an innovative membrane based on the high-performance PEBAX®2533 (PEBA) block copolymer and particles of iron-based layered double hydroxide (LDH) (MgFeAl layer composition) intercalated with phytotherapeutic abietate anions (ABI); both guest and host species are active in the promotion of wound healing. The presence of conjugated double bonds in the ABI structure promotes chemical reactions confronting its stability. Hence, LDH can protect the phytochemical species and promote its modified release. Aiming the development of wound dressings, LDH-ABI particles were immobilized in a biocompatible polymer (PEBA) by simple casting method. All samples were characterized by X-ray diffraction (XRD), vibrational (infrared and Raman) spectroscopies, thermogravimetry analysis coupled to mass spectrometry (TGA-MS), elemental chemical analyses and, in the case of polymer composites, by mechanical tests. Although the intercalation of organic anions into iron-based LDH materials is challenging, ABI intercalation was successful and using one-pot method (coprecipitation at constant pH value), according to XRD data. Additionally, spectroscopic techniques indicated the integrity of the ABI chemical structure after intercalation. The sodium abietate (NaABI) salt and the PEBA_NaABI membrane were also prepared to evaluate the effect of LDH in the formulations. In vitro release assays in saline solution at 32 °C showed the release (or solubilization) of around 3 and 5 wt./wt% of the ABI amount from LDH and salt, respectively, after 10 h. Comparatively, ABI release from the PEBA_MgFeAl-ABI and PEBA_NaABI formulations was improved to 20 and 22 wt%, respectively. The improvement in ABI release profiles from the membranes was related to the decrease in particles aggregation and improved media permeation. LDH particles released bioactive Mg cations in the saline solution and, unlike NaABI particles, also improved the mechanical performance of the polymer. Thus, PEBA_MgFeAl

In this work, Layered Double Hydroxide (LDH) materials carrying the worldwide administered non-steroidal anti-inflammatory drug naproxen (NAP), and the sodium naproxenate salt (NaNAP) for comparison, were studied by computational approaches aiming to model the structure of hybrid LDH-drug and shed light on NAP intercalation process. Atomic modeling calculations were performed at the quantum mechanical level based on Density Functional Theory and classical force fields based on empirical interatomic potentials. LDH[sbnd]NAP materials were prepared by ion exchange reaction from MgAl(OH)[sbnd]Cl and ZnAl(OH)Cl pristine phases. The characterization of the materials confirmed NAP intercalation and also the permanence of the pristine phases in the isolated materials after ion exchange. Crystallographic lattice parameters, elemental analysis, and TGA experimental results were then employed in the calculations, which revealed that NAP anions can completely neutralize the positive charge of the LDH layers: both MgAl and ZnAl LDH structures could be optimized with all Cl anions substituted by NAP. The drug assumed different dispositions in the NaNAP crystal or when intercalated into LDH. Additionally, infrared wavenumbers calculations agreed with the experimental results and showed useful to support LDH[sbnd]NAP bands assignment. The employed theoretical models to represent the structure of LDH[sbnd]NAP systems are expected to assist the interpretation of future experimental results and to be used as auxiliary tools to tune properties of LDH-drug pharmaceutical formulations.

In the last years, the use of clay minerals for pharmaceutical purposes has increased due to their interesting properties. Hectorite (Ht) is a clay belonging to the smectite group which has attracted attention for applications in biology, tissue engineering and as drug carrier and delivery system. However, the mechanisms involved in Ht cellular uptake and transport into cells, are still unclear. Herein, we used a labeled Ht (Ht/1Cl) to study both the cellular uptake, by confocal laser scanning microscopy, and internalization pathways involved in the cellular uptake, by various endocytosis-inhibiting studies and fluorescence microscopy. These studies highlighted that Ht can penetrate the cellular membrane, localizing mainly in the cytoplasm. The main intracellular transport mechanisms are the ATP-dependent ones and those where filaments and microtubules are involved. Finally, as proof of concept for the potential of Ht as carrier system, we envisaged the covalent grafting of the anticancer molecule methotrexate (MTX), chosen as model, to obtain the Ht-MTX nanomaterial. The covalent linkage was confirmed by several techniques and the morphology of the obtained nanomaterial was imaged by SEM and TEM investigations. The kinetic release of the drug from the Ht-MTX nanomaterial in physiological conditions was studied as well. Furthermore, cytotoxic studies on different cell lines, namely, HL-60, HL-60R, MCF-7, 5637, UMUC3 and RT112 showed that Ht could be a promising material for anticancer therapy.

The Aloe vera (L.) Burman f. pulp extract (AE), obtained from the inner parts of Aloe vera leaves, is rich in polysaccharides, including glucomannans, acemannans, pectic compounds, cellulose, and hemicelluloses; acemannan and glucomannan are considered the two main components responsible for most of the plant’s therapeutical properties. Besides having anti-inflammatory activity, these polysaccharides accelerate wound healing and promote skin regeneration, thus they can be utilized in healing products. The objective of this study was to develop Aloe vera mucilaginous-based hydrogels for topical use in psoriasis treatment. The hydrogels were prepared with 80% w/w of A. vera mucilaginous gel, evaluating two distinct polymers as the gelling agent: 1% carbopol 940 (FC1 and FC2) or 2% hydroxyethylcellulose (FH3 and FH4). FC1, FC2, FH3 and FH4 were evaluated for their organoleptic characteristics, rheological properties, pH and glucomannan content. Polysaccharide fractions (PFs) were extracted from the AE and used as a group of chemical markers and characterized by infrared (IR) spectroscopy and 1H nuclear magnetic resonance (H NMR). The quantification of these markers in the raw material (AE) and in the hydrogels was carried out using spectrophotometric techniques in the UV-VIS region. The hydrogels-based hydroxyethylcellulose (FH3 and FH4) had glucomannan contents of 6.76 and 4.01 mg/g, respectively. Formulations with carbopol, FC1 and FC2, had glucomannan contents of 8.69 and 9.17 mg/g, respectively, an ideal pH for application on psoriasis, in addition to good spreadability and pseudoplastic and thixotropic behavior. Considering these results, hydrogel FC1 was evaluated for its keratolytic activity in a murine model of hyperkeratinization. For that, 0.5 mL of test formulations FC1 and FPC (0.05% clobetasol propionate cream) were topically applied to the proximal region of adult rats daily for 13 days. After euthanasia, approximately 2.5 cm of the proximal portion of ea

Procedimiento de preparación de un material nanoestructurado de praziquantel y un silicato, material obtenido y uso como antiparasitario. La invención se refiere a un procedimiento de preparación de un material nanoestructurado de un silicato que tiene estructura laminar, fibrilar o tubular con praziquantel, un compuesto con actividad antiparasitaria. Otros aspectos de la invención se refieren al material obtenido mediante dicho procedimiento de preparación y al uso del mismo para la eliminación de parásitos, tanto en composiciones para el tratamiento de enfermedades parasitarias, particularmente la esquistosomiasis, como en sistemas de ventilación o conducciones de agua.

La turba, en razón de su composición, tiene un potencial empleo en el ámbito de la salud, asociado principalmente a los efectos de los ácidos húmicos y fúlvicos administrados por vía tópica. La turba se emplea como excipiente de formas semisólidas de uso en Hidrología Médica, en la formulación de peloides]. El objetivo de este trabajo ha sido estudiar la estabilidad de un sistema disperso turba/agua purificada para evaluar su posible uso en este ámbito.

Nanocomposite systems attract considerable interest in the pharmaceutic and cosmetic fields due to the wide range of advantageous properties compared to free polymers, such as the high potential to provide predictable, accurate, and reproducible patterns of controlled release and specific delivery of bioactive molecules. Studies have shown the hybridization of different clays with polymers or surfactants by strong secondary interactions of the mineral compounds with their guests. Nanostructured lipid carriers (NLC) associated with clays have gained attention in pharmaceutical areas due to their ability to transport hydrophobic drugs. Additionally, lipid-based nanoparticles are considering “nano-safety, stable, biocompatible, and have low dermal toxicity. In this context, Bixa orellana L. or “annatto,” has been proposed as a potential active ingredient in pharmaceuticals by its biological activity as healing, antioxidant, antibacterial, and anti-leishmaniasis properties. The purpose of the present study was to produce and characterize NLCs with AO in association with Laponite (L) nanoparticles (Na+ 0.7[(Si8 Mg5.5Li0.3) O20(OH)4 ]-0.7).

Uncontrolled cell proliferation is a hallmark of cancer as a result of rapid and deregulated progression through the cell cycle. The inhibition of cyclin-dependent kinases (CDKs) activities is a promising therapeutic strategy to block cell cycle of tumor cells. In this work we reported a new example of nanocomposites based on halloysite nanotubes (HNTs)/pyrazolo[3,4-d]pyrimidine derivatives (Si306 and Si113) as anticancer agents and CDK inhibitors. HNTs/Si306 and HNTs/Si113 nanocomposites were synthesized and characterized. The release kinetics were also investigated. Antitumoral activity was evaluated on three cancer cell lines (HeLa, MDA-MB-231 and HCT116) and the effects on cell cycle arrest in HCT116 cells were evaluated. Finally, molecular dynamics simulations were performed of the complexes between Si113 or Si306 and the active site of both CDK 1 and 2.

Halloysite is an aluminosilicate clay with a predominantly hollow tubular structure (HNTs) able to act as a nanocontainer for the encapsulation of several chemicals. However, HNTs possess low affinity for metal ions in their pristine form and they need to be modified for improving their adsorption capabilities. Therefore, to overcome this issue herein we report a straightforward approach for the covalent modification of the external surface of halloysite nanotubes with hectorite clay. Compared to halloysite, hectorite possesses a lamellar structure with higher cation exchange capacity. The covalent linkage between the two clays was verified by several techniques (FTIR spectroscopy,13 C CP¿MAS NMR, TGA, ¿-potential, DLS, and XRD measurements) and the morphology was imaged by TEM investigations. As proof of concept the adsorption ability of the obtained nanomaterial in comparison to pristine clays was proved using ciprofloxacin and silver ions chosen as models for their different chemical characteristics.

La invención se refiere a un procedimiento de preparación de un material nanoestructurado de un silicato que tiene estructura laminar, fibrilar o tubular con praziquantel, un compuesto con actividad antiparasitaria. Otros aspectos de la invención se refieren al material obtenido mediante dicho procedimiento de preparación y al uso del mismo para la eliminación de parásitos, tanto en composiciones para el tratamiento de enfermedades parasitarias, particularmente la esquistosomiasis, como en sistemas de ventilación o conducciones de agua. [ES], The invention relates to a method for preparing a nano-structured material of a silicate having a laminar, fibrilar or tubular structure with praziquantel, a compound with antiparasitic activity. Other aspects of the invention relate to the material obtained using the preparation method and to the use of same to eliminate parasites, both in compositions for treating parasitic diseases, particularly schistosomiasis, and in ventilation systems or water pipelines. [EN]

Hydrochlorothiazide (HCT), a Biopharmaceutical Classification System (BCS) class IV drug, is characterized by low solubility and permeability, that negatively affect its oral bioavailability, reducing its therapeutic efficacy. The combined use of cyclodextrins (CDs) and nanoclays (NCs) recently proved to be a successful strategy in developing delivery systems able to merge the potential benefits of both carriers. In this work, several binary systems of CDs or NCs with the drug were obtained, using different drug:carrier ratios and preparation techniques, and characterized in solution and in solid state, to properly select the most effective system and preparation method. Then, the best CD (RAMEB) and NC (sepiolite), at the best drug:carrier ratio, was selected for preparation of the ternary system by co-evaporation and emerged as the most effective preparation method. The combined presence of RAMEB and sepiolite gave rise to a synergistic improvement of drug dissolution properties, with a two-fold increase in the amount of drug dissolved as compared with the corresponding HCT-RAMEB system, resulting in an approximately 12-fold increase in drug solubility as compared with the drug alone. The ternary system that was co-evaporated was then selected for a tablet formulation. The obtained tablets were fully characterized for technological properties and clearly revealed a better drug dissolution performance than the commercial reference tablet (Esidrex®).