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As a prominent class of 2D transition metal dichalcogenides (TMDCs), niobium diselenide nanosheets (NbSe

A reliable surface-enhanced Raman scattering (SERS) substrate composed of two-dimensional (2D) MXene (Ti3C2Tx) nanosheets and gold nanorods (AuNRs) is designed and fabricated for sensitive detection of organic pollutants. The AuNRs are uniformly distributed on the surface of the 2D MXene nanosheets because of the strong electrostatic interactions, forming abundant SERS hot spots. The MXene/AuNR SERS substrate exhibits high sensitivity and excellent reproducibility in the determination of common organic dyes such as rhodamine 6G, crystal violet, and malachite green. The detection limits are 1 × 10-12, 1 × 10-12, and 1 × 10-10 M, and relative standard deviations determined from 13 areas on each sample are 18.1, 10.1, and 15.6%, respectively. In the determination of more complex organic pesticides and pollutants, the substrate also shows excellent sensitivity and quantitative detection, and the detection limits for thiram and diquat of 1 × 10-10 and 1 × 10-8 M, respectively, are much lower than the contaminant levels stipulated by the US Environmental Protection Agency. The MXene/AuNR composite constitutes an efficient SERS platform for reliable and high-sensitivity environmental analysis and food safety monitoring.

Black phosphorus (BP) is a promising theranostic agent owing to its excellent photothermal property, biocompatibility and biodegradability. However, the rapid degradation of BP with oxygen and moisture causes the innate instability that is the Achilles’ heel of BP, hindering its further applications in cancer theranostics. Herein, a facile surface passivation strategy was developed to prepare polydopamine (PDA) coated BP quantum dots (QDs) (denoted as BP@PDA) through self-polymerization method. PDA with enriched phenol groups plays as a scavenger of reactive oxygen, which can efficiently prevent the oxidation of BP quantum dots and make them much stable in water (∼90% for BP@PDA vs. only 10% for pure BP QDs after 10 days storage). Furthermore, PDA with strong near-infrared (NIR) absorption could greatly improve the photothermal conversion efficiency (PCE) of BP QDs from 22.6% to 64.2% (∼2.84-fold higher). Considering the excellent biodegradability and good biocompability of both BP QDs and PDA, the as-prepared BP@PDA hold great potential for cancer theranostics.

Citric acid (CA) was used in a thermally induced phase separation (TIPS) process to improve the surface hydrophilicity and cell affinity of PLLA nano-fibrous scaffolds. The evolution of architecture, structure and physicochemical properties of the scaffold after modification has been investigated. Cell viability, adhesion, proliferation and osteogenic differentiation were characterized to evaluate the cytocompatibility and biological properties of PLLA nano-fibrous scaffolds. Citric acid interacted with PLLA through hydrogen bond association and the introduction of strong polar groups (–COOH) on the PLLA surface improved its hydrophilicity with the contact angle decreasing to a suitable range for cell adhesion and spreading. The cell exhibited extensive spreading on the CA modified PLLA scaffolds with many cellular protrusions interacting with nanofibers. Furthermore, such a modification significantly increased the cell proliferation rate, enhanced the alkaline phosphatase (ALP) activity and bone-related gene expression (ALP, OCN, COL I and Runx2) of mBMSCs along with cell development. The results demonstrate a promising modification method to promote applications of PLLA-based scaffolds.

A near-infrared (NIR) light-triggered drug delivery platform is produced by incorporating SrCl2 and BP nanosheets (BPs) into poly(lactic-co-glycolic acid) (PLGA) for bone regeneration. The fabricated BP-SrCl2/PLGA microspheres show efficient NIR absorption and photothermal effects due to the BPs. The NIR-triggered release behavior of Sr2+ by flawing the PLGA shells is investigated and the microspheres exhibit excellent cell viability and biodegradability. Implantation of the BP-SrCl2/PLGA microspheres into a rat femoral defect demonstrates good tissue compatibility and excellent bone regeneration capacity under NIR light irradiation. Our study indicates that local release of Sr2+ at optimal time periods controlled by NIR irradiation improves bone regeneration significantly and this NIR-triggered drug delivery system composed of BPs is suitable for therapies requiring precise control at specific time.

In this paper, we propose a new shape memory polymer (SMP) composite with excellent near-infrared (NIR)-photoresponsive shape memory performance and biodegradability. The composite is fabricated by using piperazine-based polyurethane (PU) as thermo-responsive SMP incorporated with black-phosphorus (BP) sheets as NIR photothermal nanofillers. Under 808 nm light irradiation, the incorporated BP sheets with concentration of only 0.08 wt% enable rapid temperature increase over the glass temperature of PU and trigger the shape change of the composite with shape recovery rate of ∼100%. The in vitro and in vivo toxicity examinations demonstrate the good biocompatibility of the PU/BP composite, and it degrades naturally into non-toxic carbon dioxide and water from PU and non-toxic phosphate from BP. By implanting PU/BP columns into back subcutis and vagina of mice, they exhibit excellent shape memory activity to change their shape quickly under moderate 808 nm light irradiaiton. Such SMP composite enable the development of intelligent implantable devices, which can be easily controlled by the remote NIR light and degrade gradually after performing the designed functions in the body.

Near-infrared (NIR) light-responsive shape-memory composites have shown great potential in various biomedical applications due to their amazing remote actuation property. However, most of them are bioinert and restricted in NIR-I biological window. Here, we developed a new biodegradable NIR-II-responsive shape memory composite by the incorporation of CaSiCu4O10 nanosheets (CUP NSs) into shape memory polymer of poly (D, L-lactide-co-trimethylene carbonate) (PDLLA-co-TMC, denoted as PT). The as-prepared CUP/PT composites possessed outstanding shape memory performance upon low power NIR-II laser irradiation (1064 nm, 0.4 W·cm−2), offering the possibility of deep-tissue applications. Moreover, due to the sustained release of bioactive Cu2+ and SiO44- ions, the composites exhibited strong stimulation of angiogenesis both in vitro and in vivo. Our work demonstrated the promising potential of CUP/PT composites as NIR-II light-responsive biomaterials with enhanced tissue reconstruction ability, especially for wound healing.

One of the clinical challenges facing photothermal cancer therapy is health risks imposed by the photothermal nanoagents in vivo. Herein, a photothermal therapy (PTT) platform composed of a 2D material-based nanofibrous membrane as the agent to deliver thermal energy to tumors under near-infrared (NIR) light irradiation is described. The photothermal membrane, which is fabricated by an electrospinning poly(l-lactic acid) (PLLA) nanofibrous membrane loaded with bismuth selenide (Bi2Se3) nanoplates, exhibits very high photothermal conversion efficiency and long-term stability. Cell experiments and hematological analyses demonstrate that the Bi2Se3/PLLA membranes have excellent biocompatibility and low toxicity. PTT experiments performed in vivo with the Bi2Se3/PLLA membrane covering the tumor and NIR irradiation produce local hyperthermia to ablate the tumor with high efficiency. Different from the traditional systematical and local injection techniques, this membrane-based PTT platform is promising in photothermal cancer therapy, especially suitable for the treatment of multiple solid tumors or skin cancers, and long-term prevention of cancer recurrence after surgery or PTT, while eliminating the health hazards of nanoagents.

Two of the challenges for clinical implementation of nano-therapeutic strategies are optimization of tumor targeting and clearance of the nanoagents in vivo. Herein, a cell-mediated therapy by transporting 2D Bi2Se3 nanosheets within macrophage vehicles is described. The Bi2Se3 nanosheets with excellent near-infrared photothermal performance exhibit high macrophage uptake and negligible cytotoxicity thus facilitating the fabrication of Bi2Se3-laden-macrophages. Compared with bare Bi2Se3, the Bi2Se3-laden-macrophages after intravenous injection show prolonged blood circulation and can overcome the hypoxia-associated drug delivery barrier to target the tumor efficiently and dramatically enhance the efficiency of photothermal cancer therapy. The Bi2Se3-laden-macrophages possess good biocompatibility as demonstrated by the biochemical and histological analyses and furthermore, most of the materials are excreted from the body within 25 days. Our findings reveal a desirable system for highly efficient near-infrared photothermal cancer therapy.

Bi2Se3 has been widely used as a promising photothermal and photoacoustic agent recently. Herein, two-dimensional (2D) Bi2Se3 nanosheets with different sizes of about 30 nm (Bi2Se3-30) and 80 nm (Bi2Se3-80) have been successfully synthesized via solution-based methods. Both of the Bi2Se3 nanosheets possess high near-infrared (NIR) optical absorption, efficient photothermal conversion and excellent photoacoustic behaviors. Meanwhile, the Bi2Se3-30 nanosheets perform better. These results indicate the smaller Bi2Se3 nanosheets are more promising for optical diagnostic and photothermal therapy.

As new 2D layered nanomaterials, Bi

A reliable surface-enhanced Raman scattering (SERS) substrate composed of two-dimensional (2D) MXene (Ti

In breast cancer chemophotothermal therapy, it is a great challenge for the development of multifunctional nanoagents for precision targeting and the effective treatment of tumors, especially for metastasis. Herein, we successfully design and synthesize a multifunctional black phosphorus (BP)-based nanoagent, BP/DTX@PLGA, to address this challenge. In this composite nanoagent, BP quantum dots (BPQDs) are loaded into poly(lactic-co-glycolic acid) (PLGA) with additional conjugation of a chemotherapeutic agent, docetaxel (DTX). The in vivo distribution results demonstrate that BP/DTX@PLGA shows striking tropism for targeting both primary tumors and lung metastatic tumors. Moreover, BP/DTX@PLGA exhibits outstanding controllable chemophotothermal combinatory therapeutics, which dramatically improves the efficacy of photothermal tumor ablation when combined with near-light irradiation. Mechanistically, accelerated DTX release from the nanocomplex upon heating and thermal treatment per se synergistically incurs apoptosis-dependent cell death, resulting in the elimination of lung metastasis. Meanwhile, in vitro and in vivo results further confirm that BP/DTX@PLGA possesses good biocompatibility. This study provides a promising BP-based multimodal nanoagent to constrain cancer metastasis.

Photothermal therapy (PTT) offers many advantages such as high efficiency and minimal invasiveness, but clinical adoption of PTT nanoagents have been stifled by unresolved concerns such as the biodegradability as well as long-term toxicity. Herein, poly (lactic-co-glycolic acid) (PLGA) loaded with black phosphorus quantum dots (BPQDs) is processed by an emulsion method to produce biodegradable BPQDs/PLGA nanospheres. The hydrophobic PLGA not only isolates the interior BPQDs from oxygen and water to enhance the photothermal stability, but also control the degradation rate of the BPQDs. The in vitro and in vivo experiments demonstrate that the BPQDs/PLGA nanospheres have inappreciable toxicity and good biocompatibility, and possess excellent PTT efficiency and tumour targeting ability as evidenced by highly efficient tumour ablation under near infrared (NIR) laser illumination. These BP-based nanospheres combine biodegradability and biocompatibility with high PTT efficiency, thus promising high clinical potential., Black phosphorus is a biodegradable 2D material that has attracted growing interest in biomedicine. Here, the authors carry out in vitro and in vivo experiments to demonstrate that nanospheres loaded with black-phosphorus quantum dots perform as promising phothermal cancer therapy agents.

Poly(vinylpyrrolidone)-encapsulated Bi2 Se3 nanosheets with a thickness of 1.7 nm and diameter of 31.4 nm are prepared by a solution method. Possessing an extinction coefficient of 11.5 L g(-1) cm(-1) at 808 nm, the ultrathin Bi2 Se3 nanosheets boast a high photothermal conversion efficiency of 34.6% and excellent photoacoustic performance. After systemic administration, the Bi2 Se3 nanosheets with the proper size and surface properties accumulate passively in tumors enabling efficient photoacoustic imaging of the entire tumors to facilitate photothermal cancer therapy. In vivo biodistribution studies reveal that they are expelled from the body efficiently after 30 d. The ultrathin Bi2 Se3 nanosheets have large clinical potential as metabolizable near-infrared-triggered theranostic agents.

A titanium sulfonate ligand is synthesized for surface coordination of black phosphorus (BP). In contrast to serious degradation observed from the bare BP, the BP after surface coordination exhibits excellent stability during dispersion in water and exposure to air for a long period of time, thereby significantly extending the lifetime and spurring broader application of BP.

A simple and efficient pen-on-paper approach is designed to prepare hydrophilic surface enhanced Raman scattering (SERS)-active lines by directly writing on a piece of hydrophobic poly (L-lactic acid) nanofibrous paper using a pen filled with plasmonic nanoparticle ink. The pen-on-paper-line SERS substrate exhibits hydrophobic–hydrophilic focusing effects together with negligible background interference, high sensitivity, good reproducibility, and long-term stability. Furthermore, just by drawing three different plasmonic nanoparticles, the SERS activity is optimized for different molecules. Considering the complex factors involved in SERS effects of real analytes, our results provide an efficient strategy to produce optimized SERS substrates with multiple plasmonic nanoparticles. Copyright © 2016 John Wiley & Sons, Ltd.

As a prominent member of two dimensional (2D) materials, MXenes have shown encouraging photophysical properties and so there is highly desirability to explore their phototherapeutic potential in cancer. Herein, we demonstrate a facile top-down strategy for the synthesis of nitride-based MXene, titanium nitride quantum dots (Ti2N QDs) in solution. With a size of around 5 nm, the obtained Ti2N QDs exhibit extraordinarily high photothermal conversion efficiency under laser irradiation in both first and second near-infrared (NIR) biowindows (NIR-I, 808 nm, 48.62%; and NIR-II, 1064 nm, 45.51%). In vitro and in vivo assessments demonstrate that the Ti2N QDs possess excellent biocompatibility, photoacoustic (PA) effect, and photothermal therapy (PTT) efficiency. Moreover, the Ti2N QDs showing obvious aggregation in tumors after 4 h post-injection, which enables facilitate PA imaging-guided PTT in both NIR-I/II biowindows without noticeable toxicity. Encouragingly, the Ti2N QDs with appropriate degradation property also show an applicable excretion rate from the body in vivo, which ensures sufficient stability in circulation to accomplish therapeutics roles and then can be smoothly discharged from the body after that. These results indicate the high potential of biodegradable Ti2N QDs in PA imaging-guided PTT in both NIR-I/II biowindows for precision cancer treatment.

Although phosphorene has attracted much attention in electronics and optoelectronics as a new type of two-dimensional material, in-depth investigations and applications have been limited by the current synthesis techniques. Herein, a basic N-methyl-2-pyrrolidone (NMP) liquid exfoliation method is described to produce phosphorene with excellent water stability, controllable size and layer number, as well as in high yield. Phosphorene samples composed of one to four layers exhibit layer-dependent Raman scattering characteristics thus providing a fast and efficient means for the in situ determination of the thickness (layer number) of phosphorene. The linear and nonlinear ultrafast absorption behavior of the as-exfoliated phosphorene is investigated systematically by UV–vis–NIR absorption and Z-scan measurements. By taking advantage of their unique nonlinear absorption, ultrashort pulse generation applicable to optical saturable absorbers is demonstrated. In addition to a unique fabrication technique, our work also reveals the large potential of phosphorene in ultrafast photonics.

Photothermal therapy (PTT) is a fledgling therapeutic strategy for cancer treatment with minimal invasiveness but clinical adoption has been stifled by concerns such as insufficient biodegradability of the PTT agents and lack of an efficient delivery system. Here, black phosphorus (BP) nanosheets are incorporated with a thermosensitive hydrogel [poly(d,l‐lactide)‐poly(ethylene glycol)‐poly(d,l‐lactide) (PDLLA‐PEG‐PDLLA: PLEL)] to produce a new PTT system for postoperative treatment of cancer. The BP@PLEL hydrogel exhibits excellent near infrared (NIR) photothermal performance and a rapid NIR‐induced sol–gel transition as well as good biodegradability and biocompatibility in vitro and in vivo. Based on these merits, an in vivo PTT postoperative treatment strategy is established. Under NIR irradiation, the sprayed BP@PLEL hydrogel enables rapid gelation forming a gelled membrane on wounds and offers high PTT efficacy to eliminate residual tumor tissues after tumor removal surgery. Furthermore, the good photothermal antibacterial performance prevents infection and this efficient and biodegradable PTT system is very promising in postoperative treatment of cancer.

Atomic force microscopy (AFM) technique was used to investigate the nanomechanical properties of poly(l-lactide) (PLLA) nanofibers produced by the thermally induced phase separation (TIPS) method. Firstly, AFM-based nanolithography was employed to produce localized deformations on the surface of single PLLA nanofiber, in which the AFM tip served as a nanoscale burin to draw a scratch longitudinally along the nanofiber. Secondly, the morphology and physical properties of the nanofiber before and immediately after the deformation were characterized with AFM and force spectroscopy measurement. During the initial stage of TIPS process, the crystallization of PLLA resulted in a regular arrangement of crystalline domains along the thinner fibrils which then assembled laterally into larger nanofibers. The deformation due to the nanoindentation and plowing with the probe induced structural variation of PLLA nanofibers and led to a functional consequence in their nanomechanical properties. The region after deformation had a higher adhesion force and elastic modulus, probably because the polymer chains became more compact and ordered under both compression and shear stresses.

This study aimed to investigate the variation of structure and nanomechanical properties of human articular cartilage (AC) at different stages of osteoarthritis (OA). The nanoscale morphology, chemical composition, variation of chemical structure, surface adhesion force and elastic modulus were examined. The thickening of collagen fibrils and a decreasing trend of their D-periodic banding patterns were observed along with the progression of OA. The calcium and phosphate concentration in AC showed an increasing trend from Grade 0 to Grade 3. These findings suggest that collagen fibrils have reduced intermolecular interactions, greater molecular disorder and decreased amount and stability of crosslinks in collagen, which may affect the stability of collagen fibrils. The surface adhesion force showed a decreasing trend while the elastic modulus of individual collagen fibrils showed an increasing trend with the advancement of OA, which was confirmed to have a direct functional consequence in the nanostructure of collagen fibrils. This study is helpful for understanding OA pathogenesis and providing an efficient strategy for pre-symptomatic diagnostics of OA.

As new 2D layered nanomaterials, Bi2 O2 Se nanoplates have unique semiconducting properties that can benefit biomedical applications. Herein, a facile top-down approach for the synthesis of Bi2 O2 Se quantum dots (QDs) in a solution is described. The Bi2 O2 Se QDs with a size of 3.8 nm and thickness of 1.9 nm exhibit a high photothermal conversion coefficient of 35.7% and good photothermal stability. In vitro and in vivo assessments demonstrate that the Bi2 O2 Se QDs possess excellent photoacoustic (PA) performance and photothermal therapy (PTT) efficiency. After systemic administration, the Bi2 O2 Se QDs accumulate passively in tumors enabling efficient PA imaging of the entire tumors to facilitate imaging-guided PTT without obvious toxicity. Furthermore, the Bi2 O2 Se QDs which exhibit degradability in aqueous media not only have sufficient stability during in vivo circulation to perform the designed therapeutic functions, but also can be discharged harmlessly from the body afterward. The results reveal the great potential of Bi2 O2 Se QDs as a biodegradable multifunctional agent in medical applications.

Self-assembled monolayers with different terminal chemical groups including thiol ( SH), methyl ( CH3), carboxyl ( COOH) and hydroxyl ( OH) were employed as substrates for the culture of hepatoma cells (HepG2s). X-ray photoelectron spectroscopy and atomic force microscopy confirmed the similar density of different functional groups occupation. The adhesion and proliferation of cancer cells exhibited significant difference on different surfaces. The HepG2s adhered to CH3 surfaces but exhibited the smallest contact area with mostly rounded morphology, while those on SH surfaces exhibited the largest contact area with extensive spreading. The proliferation of HepG2s in prolonged culture was significantly inhibited on CH3 surface. Cells on other surfaces of various chemical groups proliferated at different levels. After 7 days of culture, the proliferation of HepG2s on the different surfaces followed the trend: OH ≈ COOH > SH ≫ CH3. Due to the strong hydrophobic property, the CH3 group inhibited the cell adhesion, which led to the death of cancer cells. Compared with other chemical functional groups, the CH3 group exhibited its unique effect on the fate of cancer cells, providing a potential way on prevention and treatment of liver cancer.

The nonlinear optical property of topological insulator bismuth selenide (Bi2Se3) is found to be well-tailored through ion irradiation by intentionally introducing defects. The increase of the optical modulation depth sensitively depends on the careful selection of the irradiation condition. By implementing the ion irradiated Bi2Se3 film as an optical saturable absorber device for the Q-switched wave-guide laser, an enhanced laser performance has been obtained including narrower pulse duration and higher peak power. Our work provides a new approach of tailoring the nonlinear optical properties of materials through ion irradiation, a well-developed chip-technology, which could find wider applicability to other layered two-dimensional materials beyond topological insulators, such as graphene, MoS2, black phosphours etc.

The surface morphology, crystalline structure and nanomechanical properties of poly( l -lactide) (PLLA) samples prepared via thermally induced phase separation (TIPS) process have been investigated by scanning electron microscopy (SEM), attenuated total reflection-Fourier transform infrared spectroscopy (ATR-FTIR), wide-angle X-ray diffraction (WAXD), atomic force microscopy (AFM), force spectroscopy and nanoindentation. Typical nanofibrous scaffold was obtained at −24 °C (NF sample) while a denser matrix with some plateletlike structure was obtained at 15 °C (PL sample). The NF sample has a higher crystallinity with α′-form crystals while the PL sample has α-form crystals embedded in a largely amorphous matrix. The two kinds of samples have differences in the chain conformation with a more restricted backbone vibration and stiffened segmental motion in NF samples. The NF samples have a higher adhesion force although both samples showed a heterogeneous distribution of adhesion force on the surface based on force spectroscopy analysis. The alternating distribution of domains with higher and lower adhesion force exhibited a banded pattern on PLLA nanofibre. This pattern is proposed to reflect the distribution of crystal-rich and amorphous-rich domains in the semicrystalline samples. AFM-based nanoindentation test indicated that the nanofibrous NF samples can have more significant plastic deformation and creep than the largely amorphous PL samples. The sliding of the crystal-rich domains along the fibrils would account for this increased plasticity of the nanofiber.

The structural evolution and the corresponding biodegradability and biological property of PLLA porous scaffolds during the early quenching period in a thermally induced phase separation process have been investigated. The morphology, crystallization behavior, chemical structure, surface property, hydrophobicity, biodegradability and biological property were studied by using SEM, WAXD, XPS, contact angle measurement, AFM, hydrolytic degradation and cell culture experiments. The initial phase separation resulted in an amorphous gel with the condensation of patches of amorphous precipitates, followed by the nucleation of PLLA crystals. With extending the gelation process, a microporous structure was formed. A temperature dependent phase behavior during the early quenching period has been observed. Along with the increase in the degree of crystallinity, structural transformation of the polymer toward a more ordered and compact state proceeded with the extending of the gelation time. The possible surface segregation of the methyl groups was confirmed by XPS analysis which may have certain effect on the increase of water contact angle. The evolution of architecture, crystallinity, chemical structure, surface property and the polymer chain packing mode, etc, during the early quenching period, has a direct functional consequence in the hydrophobicity, biodegradability as well as biological property.

Black phosphorus quantum dots (BPQDs) were synthesized using a liquid exfoliation method that combined probe sonication and bath sonication. With a lateral size of approximately 2.6 nm and a thickness of about 1.5 nm, the ultrasmall BPQDs exhibited an excellent NIR photothermal performance with a large extinction coefficient of 14.8 L g(-1) cm(-1) at 808 nm, a photothermal conversion efficiency of 28.4%, as well as good photostability. After PEG conjugation, the BPQDs showed enhanced stability in physiological medium, and there was no observable toxicity to different types of cells. NIR photoexcitation of the BPQDs in the presence of C6 and MCF7 cancer cells led to significant cell death, suggesting that the nanoparticles have large potential as photothermal agents.

Black phosphorus quantum dots (BPQDs) were synthesized using a liquid exfoliation method that combined probe sonication and bath sonication. With a lateral size of approximately 2.6 nm and a thickness of about 1.5 nm, the ultrasmall BPQDs exhibited an excellent NIR photothermal performance with a large extinction coefficient of 14.8 L g(-1) cm(-1) at 808 nm, a photothermal conversion efficiency of 28.4%, as well as good photostability. After PEG conjugation, the BPQDs showed enhanced stability in physiological medium, and there was no observable toxicity to different types of cells. NIR photoexcitation of the BPQDs in the presence of C6 and MCF7 cancer cells led to significant cell death, suggesting that the nanoparticles have large potential as photothermal agents.

We report a new paper-based surface enhanced Raman scattering (SERS) substrate platform contributed by a poly(l-lactic acid) (PLLA) nanofibrous paper adsorbed with plasmonic nanostructures, which can circumvent many challenges of the existing SERS substrates. This PLLA nanofibrous paper has three-dimensional porous structure, extremely clean surface with good hydrophobicity (contact angle is as high as 133.4°), and negligible background interference under Raman laser excitation. Due to the strong electrostatic interaction between PLLA nanofiber and cetyltrimethylammonium bromide (CTAB) molecules, the CTAB-coated gold nanorods (GNRs) are efficiently immobilized onto the fibers. Such a hydrophobic paper substrate with locally hydrophilic SERS-active area can confine analyte molecules and prevent the random spreading of molecules. The confinement leads to focusing effect and the GNRs-PLLA SERS substrate is found to be highly sensitive (0.1 nM Rhodamine 6G and malachite green) and exhibit excellent reproducibility (∼8% relative standard deviation (RSD)) and long-term stability. Furthermore, it is also cost-efficient, with simple fabrication methodology, and demonstrates high sample collection efficiency. All of these benefits ensure that this GNRs-PLLA substrate is a really perfect choice for a variety of SERS applications.