Severe bone defects pose a formidable clinical challenge in orthopedics, urgently demanding the development of advanced biomaterials to restore structural and functional integrity. While current regenerative materials, such as collagen-containing products, demonstrate a certain degree of biocompatibility, they are still hampered by limitations that include poor mechanical performance, restricted barrier effects, and arduous preparation methods. Here, we report a rapid-curing methodology to engineer recombinant resilin bioshield with tunable modulus, superior bioactivity, and rapid assembly kinetics. The resilin bioshield is rapidly formed within minutes via a tyrosine-mediated photo-crosslinking strategy, achieving spatially programmable assembly. Enzymatic integration of alkaline phosphatase into the resilin matrix drives in situ mineralization, yielding densely packed hydroxyapatite (HAP) nanocrystals. Remarkably, this process enables controlled modulus tuning of the bioshield across three orders of magnitude, achieving an exceptional maximum modulus of 145 MPa while retaining excellent flexibility, thus surpassing conventional guided bone regeneration materials. Beyond its mechanical superiority, the mineralized resilin bioshield not only directs cellular behavior by enhancing adhesion and spreading but also robustly drives the osteogenic differentiation of mesenchymal stem cells, thereby accelerating functional bone regeneration. As a result, our work provides an alternative approach for creating high-performance barrier membranes for guided bone regeneration.