This study proposes an innovative way of synthesizing porous gelatin/silica bioglass composite microspheres with a nanofibrous structure using emulsion coupled with thermally induced phase separation (TIPS). In particular, a mixture of the solvent (water) and non-solvent (ethanol) was used to induce a unique phase separation of gelatin/silica mixtures (i.e. gelatin/silica hybrid-rich and liquid-rich phases) at −70°C for the creation of a nanofibrous structure. All the composite microspheres synthesized with silica contents of 10wt.%, 15wt.%, and 20wt.% had well-defined spherical shapes between 124 and 136μm in size. In addition, they were comprised of nanofibrous gelatin/silica composite walls (several tens of nanometers in thickness), where the sol–gel derived silica bioglass phase was uniformly distributed throughout the gelatin matrix. The in vitro apatite-forming ability and biocompatibility of the nanofibrous gelatin/silica bioglass composite microspheres was significantly enhanced with an increase in silica content, demonstrating their great potential for the promotion of bone tissue regeneration.