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Engineered composite scaffolds composed of natural and synthetic polymers exhibit cooperation at the molecular level that closely mimics tissue extracellular matrix's (ECM) physical and chemical characteristics. However, due to the lack of smooth intermix capability of natural and synthetic materials in the solution phase, bio‐inspired composite material development has been quite challenged. In this research, we introduced new bio‐inspired material blending techniques to fabricate nanofibrous composite scaffolds of chitin nanofibrils (CNF), a natural hydrophilic biomaterial and poly (ɛ‐caprolactone) (PCL), a synthetic hydrophobic‐biopolymer. CNF was first prepared by acid hydrolysis technique and dispersed in trifluoroethanol (TFE); and second, PCL was dissolved in TFE and mixed with the chitin solution in different ratios. Electrospinning and spin‐coating technology were used to form nanofibrous mesh and films, respectively. Physicochemical properties, such as mechanical strength, and cellular compatibility, and structural parameters, such as morphology, and crystallinity, were determined. Toward the potential use of this composite materials as a support membrane in blood–brain barrier application (BBB), human umbilical vein endothelial cells (HUVECs) were cultured, and transendothelial electrical resistance (TEER) was measured. Experimental results of the composite materials with PCL/CNF ratios from 100/00 to 25/75 showed good uniformity in fiber morphology and suitable mechanical properties. They retained the excellent ECM‐like properties that mimic synthetic‐bio‐interface that has potential application in biomedical fields, particularly tissue engineering and BBB applications.

Nano-in-micro (NIM) system is a promising approach to enhance the performance of devices for a wide range of applications in disease treatment and tissue regeneration. In this study, polymeric nanofibre-integrated alginate (PNA) hydrogel microcapsules were designed using NIM technology. Various ratios of cryo-ground poly (lactide-co-glycolide) (PLGA) nanofibres (CPN) were incorporated into PNA hydrogel microcapsule. Electrostatic encapsulation method was used to incorporate living cells into the PNA microcapsules (~500 µm diameter). Human liver carcinoma cells, HepG2, were encapsulated into the microcapsules and their physio-chemical properties were studied. Morphology, stability, and chemical composition of the PNA microcapsules were analysed by light microscopy, fluorescent microscopy, scanning electron microscopy (SEM), Fourier-Transform Infrared spectroscopy (FTIR), and thermogravimetric analysis (TGA). The incorporation of CPN caused no significant changes in the morphology, size, and chemical structure of PNA microcapsules in cell culture media. Among four PNA microcapsule products (PNA-0, PNA-10, PNA-30, and PNA-50 with size 489 ± 31 µm, 480 ± 40 µm, 473 ± 51 µm and 464 ± 35 µm, respectively), PNA-10 showed overall suitability for HepG2 growth with high cellular metabolic activity, indicating that the 3D PNA-10 microcapsule could be suitable to maintain better vitality and liver-specific metabolic functions. Overall, this novel design of PNA microcapsule and the one-step method of cell encapsulation can be a versatile 3D NIM system for spontaneous generation of organoids within vivolike tissue architectures, and the system can be useful for numerous biomedical applications, especially for liver tissue engineering, cell preservation, and drug toxicity study.