Biomimetic, Stiff, and Adhesive Periosteum with Osteogenic–Angiogenic Coupling Effect for Bone Regeneration

Abstract Current periosteal grafts have limitations related to low mechanical strength, tissue adhesiveness, and poor osteogenesis and angiogenesis potential. Here, a periosteum mimicking bone aid (PMBA) with similar structure and function to natural periosteum is developed by electrospinning photocrosslinkable methacrylated gelatin (GelMA), l ‐arginine‐based unsaturated poly(ester amide) (Arg‐UPEA), and methacrylated hydroxyapatite nanoparticles (nHAMA). Such combination of materials enhances the material mechanical strength, favors the tissue adhesion, and guarantees the sustained activation of nitric oxide–cyclic guanosine monophosphate (NO–cGMP) signaling pathway, with well‐coordinated osteogenic–angiogenic coupling effect for accelerated bone regeneration. This work presents a proof‐of‐concept demonstration of thoroughly considering the progression of implant biomaterials: that is, the initial material components (i.e., GelMA, Arg‐UPEA, and nHAMA) equip the scaffold with suitable structure and function, while its degradation products (i.e., Ca 2+ and l ‐arginine) are involved in long‐term mediation of physiological activities. It is envisioned that the strategy will inspire the design of high‐performance bioscaffolds toward bone and periosteum tissue engineering.