AbstractIn this study, the novel biomimetic aerogel‐based composite scaffolds through a synergistic combination of wet chemical synthesis and advanced engineering approaches have successfully designed. To this aim, initially the photo‐crosslinkable methacrylated silk fibroin (SF‐MA) biopolymer and methacrylated hollow mesoporous silica microcapsules (HMSC‐MA) as the main constituents of the novel composite aerogels were synthesized. Afterward, by incorporation of drug‐loaded HMSC‐MA into the self‐assembled SF‐MA, printable gel‐based composite inks are developed. By exploiting micro‐extrusion‐based three‐dimensional (3D) printing, SF‐MA‐HMSC composite gels are printed by careful controlling their viscosity to provide a means to control the shape fidelity of the resulted printed gel constructs. The developed scaffold has shown a multitude of interesting biophysical and biological performances. Namely, thanks to the photo‐crosslinking of the gel components during the 3D printing, the scaffolds become mechanically more stable than the pristine SF scaffolds. Also, freeze‐casting the printed constructs generates further interconnectivity in the printed pore struts resulting in the scaffolds with hierarchically organized porosities necessary for cell infiltration and growth. Importantly, HMSC incorporated scaffolds promote antibacterial drug delivery, cellular ingrowth and proliferation, promoting osteoblastic differentiation by inducing the expression of osteogenic markers and matrix mineralization. Finally, the osteoconductive, ‐inductive, and anti‐infective composite aerogels are expected to act as excellent bone implanting materials with an extra feature of local and sustained release of drug for efficient therapy of bone‐related diseases.