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The current research attempted to address the suitability of bioactive Sambucus nigra extract entrapped in albumin-decorated nanostructured lipid carriers (NLCs) as a promising "adjuvant" in improving tumour penetration for multiple antitumour therapy. The new hybrid albumin-decorated NLCs were characterised based on, e.g., the particle size, zeta electrokinetic potential, SambucusN entrapment efficiency, and fluorescence spectroscopy and tested for different formulation parameters. The antioxidant activity of NLC- SambucusN was significantly enhanced by a bovine serum albumin (BSA) polymer coating. According to the real-time cell analysis (RTCA) results, NLC-I- SambucusN -BSA behaved similarly to the chemotherapeutic drug, cisplatin, with cell viability for LoVo tumour cells of 21.81 ± 1.18%. The new albumin-NLC- SambucusN arrested cancer cells in G1 and G2 cycles and intensified the apoptosis process in both early and late phases. An advanced induction, over 50% apoptosis in LoVo colon cells, was registered for 50 μg/mL of NLC-II- SambucusN -BSA, a fourfold increase compared to that of untreated cells. RTCA and flow cytometry results showed that concentrations of the hybrid NLC- SambucusN up to 50 μg/mL do not affect the proliferation of normal HUVEC cells. This approach provides insightful information regarding the involvement of phytochemicals in future therapeutic strategies. Albumin-decorated NLCs can be considered a noteworthy strategy to be connected to antitumour therapeutic protocols.