Guided bone regeneration (GBR) membrane has proven to be a fundamental tool in the realm of bone defect repair. In this study, we develop a mussel-inspired composite biomaterial through polydopamine-assisted, combining gelatin-WPU matrix with the ion-release behavior of Cu-MSNs for augmented bone regeneration. The optimized composite membrane exhibits enhanced mechanical stability, demonstrating a tensile strength of 11.23 MPa (representing a 2.3-fold increase compared to Bio-Gide), coupled with significantly slower degradation kinetics that retained 73.3% structural integrity after 35-day immersion in physiological solution. Copper ions act as angiogenic agents to promote blood vessel growth and as antimicrobial agents to prevent potential infections. The combined effect of these components creates a biomimetic environment that is ideal for cell adhesion, growth, and differentiation. This research significantly contributes to the development of advanced biomaterials that combine regeneration and infection-prevention functions. It provides a versatile and effective solution for treating bone injuries and defects, offering new hope for patients in need.