Patients with osteoporosis face challenges such as decreased bone density, a sparse trabecular structure, weakened osteogenic ability, and impaired angiogenesis, leading to poor osseointegration and implant failure. Surface modification of implants with biologically active molecules possessing various functions is an effective strategy to improve osseointegration. In this study, we constructed a simple multifunctional coating interface that significantly improves osseointegration. In brief, a multifunctional coating interface was constructed by coupling the Rgd adhesive peptide, Ogp osteogenic peptide, and Ang angiogenic peptide to Lys (k), which self-assembled layer by layer with TA to form the (TA-Rgd@ogp@ang)n composite membrane. This study characterized the surface morphology and biomechanical properties of the coating under both gas and liquid phases and monitored the deposition process and reaction rate of the two peptides with TA using a quartz crystal microbalance. Moreover, (TA-Rgd@ogp@ang)n exhibited a triple synergistic effect on cell migration and adhesion, osteogenic differentiation, and angiogenesis. It also ameliorated the high ROS environment characteristic of osteoporosis pathology, promoted angiogenic bone defect regeneration in osteoporosis, thereby avoiding poor osseointegration. This work provides a new approach for the prevention of implant failure in pathological environments by constructing multifunctional coatings on implants, with tremendous potential applications in the fields of orthopedics and dentistry.