Bone regeneration remains a critical challenge in regenerative medicine, particularly in dentistry, where conditions such as periodontal disease and trauma can lead to significant bone defects. Traditional treatment methods, such as autogenous bone grafting, face limitations, including donor site morbidity and postoperative complications. Recent advancements in biomaterials, particularly silk fibroin-based scaffolds, have shown promise due to their excellent biocompatibility and tunable mechanical properties. Incorporating bioactive glass and metal ions, such as cobalt, into these scaffolds can enhance osteogenic properties and antibacterial effects, creating an optimal environment for bone regeneration. The primary objective of this study was to develop and characterize SilkMA/silicated-chlorinated cobalt-doped bioactive glass composites with the potential for bone regeneration applications. Utilizing the sol-gel method, we synthesized cobalt-doped bioglass, enhancing its bioactivity and antibacterial properties. Mechanical testing, swelling assessments, degradation analysis, and in vitro evaluations using alveolar bone-derived mesenchymal stem cells (aBMSCs) demonstrated the scaffolds' cytocompatibility and favorable physical properties. The structural integrity of the electrospun fibers was confirmed through Scanning Electron Microscopy (SEM), Fourier Transform Infrared Spectroscopy (FTIR), and Raman Spectroscopy analyses. Incorporating bioglass reduced swelling ratios, while in vitro assays showed that cobalt ions effectively inhibited the biofilm formation of Porphyromonas gingivalis. In vivo analysis using hematoxylin-eosin and von Kossa (vK) staining demonstrated that the SilkMA + 20% BGCo scaffold elicited a minimal inflammatory response, confirming its biocompatibility. However, the absence of positively stained structures in the vK analysis indicated its lack of mineralization potential. In sum, SilkMA/BGCo scaffolds showed promising in vitro potential for bone tissue regeneration and excellent biocompatibility in vivo despite lacking calcium deposition. Further studies with alternative in vivo models are needed to confirm their efficacy.