This study aimed to synthesize bioactive glass (BG) and phosphorylated chitosan (PCS), and fabricate a BG/PCS composite scaffold. The physical properties (mechanical strength, swelling degree, and degradation rate) of the BG/PCS scaffold were tested. The in vitro mineralization properties of composite scaffolds in simulated body fluid were investigated. MC3T3-E1 cell responses with the BG/PCS scaffold were investigated using live/dead cell staining, actin staining, alkaline phosphatase (ALP) activity, and Alizarin red staining (ARS). Our results showed that the scaffold had an inner porous structure, good swelling properties, and good degradation rate. After immersion in SBF, the scaffolds demonstrated high properties in inducing mineralization. Leaching solutions of the composite scaffolds exhibited good cytocompatibility. MC3T3-E1 cells adhered, spread, and proliferated on the scaffold. The BG/PCS composite scaffold showed osteo-inductive activity by increasing alkaline phosphatase activity and calcium deposition. Our results indicated that the BG/PCS scaffold had potential applications as a bone-defect repair biomaterial.