Given the exponential growth of the recombinant human collagen market, it is paramount to devise a robust and straightforward design strategy aimed at preserving the remarkable biological activity of recombinant human collagen while endowing it with tailored mechanical properties and stable morphologies. This innovative approach stands to broaden its applicability in hard tissue repair endeavors. Our study employed a synergistic approach of alkali hydrolysis and Schiff's base chemistry to graft Type I recombinant human collagen (rhCol-I) onto poly (L-lactic acid) (PLLA) membranes, yielding PLLA-rhCol composites. In vitro evaluations substantiated that this reengineered material not only retained the biological efficacy of rhCol-I but also imparted mechanical robustness and processability ideal for bone implant applications. Notably, it exhibited superior tissue engineering attributes, fostering proliferation, adhesion, osteogenic differentiation, mineralization of bone marrow mesenchymal stem cells (BMSCs), and encouraging vascularization. In a rat model of critical-sized bone defects, PLLA-rhCol exhibited markedly enhanced bone repair efficiency over conventional PLLA bone implants, achieving a bone volume fraction (BV/TV) of up to 32.57 ± 3.77 %, while promoting angiogenesis and effectively mitigating inflammatory cell infiltration. This pioneering method of modifying recombinant human collagen onto the side chains of polymeric macromolecules portends broad applicability in enhancing various biocompatible, yet mechanically robust and processable polymers, thereby expanding the horizons of recombinant human collagen utilization in tissue engineering and catering to the ever-evolving market demands.