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Malignant osteosarcoma is one of the serious health concerns attributed to inferior prognosis and uncontrolled metastasis in clinics. Indeed, multifunctional therapeutics with precise tumor killing and subsequent regeneration of damaged tissue are of immense requirement in treating osteosarcoma. Herein, this study demonstrates the fabrication of versatile calcium/copper-impregnated bioactive glass (Ca-BG/Cu-BG) frameworks with orchestrated cancer inhibition and bone tissue calcification towards osteosarcoma therapy. Initially, the designed composites are systematically characterized to explore various morphological attributes and physicochemical properties. The optimal formulation of Cu-BG (10 mol%) presented orchestrated effects of an excellent pH-responsive anticancer effect through hydroxyl radical (·OH) generation and facilitated hydroxyapatite formation towards bone tissue calcification. Further, in …