Bioactive glass (BG) represents a promising biomaterial for bone healing; here injectable BG pastes biological properties were improved by the addition of gelatin or chitosan, as well as mechanical resistance was enhanced by adding 10 or 20 wt% 3-Glycidyloxypropyl trimethoxysilane (GPTMS) cross-linker. Composite pastes exhibited bioactivity as apatite formation was observed by Scanning Electron Microscopy (SEM) and X-Ray Diffraction (XRD) after 14 days immersion in simulated body fluid (SBF); moreover, polymers did not enhance degradability as weight loss was >10% after 30 days in physiological conditions. BG-gelatin-20 wt% GPTMS composites demonstrated the highest compressive strength (4.8 ± 0.5 MPa) in comparison with the bulk control paste made of 100% BG in water (1.9 ± 0.1 MPa). Cytocompatibility was demonstrated towards human mesenchymal stem cells (hMSC), osteoblasts progenitors, and endothelial cells. The presence of 20 wt% GPTMS conferred antibacterial properties thus inhibiting the joint pathogens Staphylococcus aureus and Staphylococcus epidermidis infection. Finally, hMSC osteogenesis was successfully supported in a 3D model as demonstrated by alkaline phosphatase release and osteogenic genes expression.