Bone disorders caused by traumatism or diseases may lead to severe complications of the neuromuscular system. Advanced tools and technologies have been developed for bone tissue regeneration. Functional materials such as biopolymers and bioresorbable fillers have gained particular attention, owing to their ability to promote cell adhesion, proliferation and extracellular matrix production, promoting new bone ingrowth [1,2]. In this study, novel biocomposites for bone regeneration composed by β-tricalcium phosphate (β-TCP) incorporating Zn, Sr, and Mn, and silk fibroin (SF) were successfully developed. Ionic-doped biomaterials can enhance osteogenesis and angiogenesis while may help tuning the host healing response at the site of injury, and can also improve their mechanical strength.