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The majority of chitosan-based bone tissue engineering (BTE) scaffolds have the problem of poor mechanical properties. However, modifying chitosan with conventional silane coupling agents to improve the mechanical properties of scaffolds will introduce additional complications, including cytotoxicity and poor biocompatibility. In this study, two types of organic−inorganic composite scaffolds (F-A-T0/T3/T5 and F-B-T5-P0/P0.5/P1.5/P2.5) were prepared using chitosan nanofibers (CSNF) prepared by the beating-homogenization method, combined with the sol−gel method, and further introduced polyvinyl alcohol (PVA). The F-A-T3 and F-B-T5-P1.5 exhibited interconnected pore and surface nanofibers structures, high porosity (>70%), outstanding swelling properties, and a controllable degradation rate. The Young’s modulus of TEOS: 5.0% (w/w), PVA: 1.5% (w/w) chitosan fiber scaffold is 8.53 ± 0.43 MPa in dry conditions, and 237.78 ± 8.86 kPa in wet conditions, which is four times that of F-A-T5 and twice that of F-B-T5-P0. Additionally, cell (MC3T3-E1) experiments confirmed that the two composite scaffolds had great cytocompatibility and were predicted to be used in the future in the field of BTE scaffolds.