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Three-dimensional (3D) printing was utilized for the fabrication of a composite scaffold of poly(ε-caprolactone) (PCL) and calcium magnesium phosphate (CMP) bioceramics for bone tissue engineering application. Four groups of scaffolds, that is, PMC-0, PMC-5, PMC-10, and PMC-15, were fabricated using a custom 3D printer. Rheology analysis, surface morphology, and wettability of the scaffolds were characterized. The PMC-0 scaffolds displayed a smoother surface texture and an increase in the ceramic content of the composite scaffolds exhibited a rougher structure. The hydrophilicity of the composite scaffold was significantly enhanced compared to the control PMC-0. The effect of ceramic content on the bioactivity of fibroblast NIH/3T3 cells in the composite scaffold was investigated. Cell viability and toxicity studies were evaluated by comparing results from lactate dehydrogenase (LDH) and Alamar Blue (AB) colorimetric assays, respectively. The live-dead cell assay illustrated the biocompatibility of the tested samples with more than 100% of live cells on day 3 compared to the control one. The LDH release indicated that the composite scaffolds improved cell attachment and proliferation. In this research, the fabrication of a customized composite 3D scaffold not only mimics the rough textured architecture, porosity, and chemical composition of natural bone tissue matrices but also serves as a source for soluble ions of calcium and magnesium that are favorable for bone cells to grow. These 3D-printed scaffolds thus provide a desirable microenvironment to facilitate biomineralization and could be a new effective approach for preparing constructs suitable for bone tissue engineering. 

Abstract 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.