Current approaches to develop bone tissue engineering scaffolds have some limitations and shortcomings. They mainly suffer from combining mechanical stability and bioactivity on the same platform. Synthetic polymers are able to produce mechanically stable sturctures with fibrous morphology when they are electrospun, however, they cannot exhibit bioactivity, which is crucial for tissue engineering and regenerative medicine. One current strategy to bring bioactivity in synthetic materials is to combine extracellular matrix (ECM)-sourced materials with biologically inert synthetic materials. ECM-sourced materials without any modifications are mechanically unstable; therefore, reinforcing them with mechanically stable platforms is indispensable. In order to overcome this bifacial problem, we have demonstrated that poly(butylene adipate-co-terephthalate) (PBAT) electrospun microfibrous membranes can be successfully modified with decellularized bone ECM to endow fibers with bioactive hydrogel and mimic natural micro-features of the native bone tissue. The developed structures have been shown to support osteogenesis, confirmed by histochemical staining and gene expression studies. Furthermore, ECM-coated PBAT fibers, when they were aligned, supplied an improved level of osteogenesis. The strategy demonstrated can be adapted to any other tissues, and the emerging microfibrous, mechanically stable, and bioactive materials can find implications in the specific fields of tissue engineering and regenerative medicine.