Polyetheretherketone (PEEK) is a biocompatible polymer, but its clinical application is largely limited due to its inert surface. To solve this problem, a multifunctional PEEK implant is urgently fabricated. In this work, a dual-metal−organic framework (Zn−Mg-MOF74) coating is bonded to PEEK using a mussel-inspired polydopamine interlayer to prepare the coating, and then, dexamethasone (DEX) is loaded on the coating surface. The PEEK surface with the multifunctional coating provides superior hydrophilicity and favorable stability and forms an alkaline microenvironment when Mg 2+ , Zn 2+ , 2,5-dihydroxyterephthalic acid, and DEX are released due to the coating degradation. In vitro results showed that the multifunctional coating has strong antibacterial ability against both Escherichia coli and Staphylococcus aureus; it also improves human umbilical vein endothelial cell angiogenic ability and enhances rat bone marrow mesenchymal stem cell osteogenic differentiation activity. Furthermore, the in vivo rat subcutaneous infection model, chicken chorioallantoic membrane model, and rat femoral drilling model verify that the PEEK implant coated with the multifunctional coating has strong antibacterial and angiogenic ability and promotes the formation of new bone around the implant with a stronger bone−implant interface. Our findings indicate that DEX loaded on the Zn−Mg-MOF74 coating-modified PEEK implant with bacteriostasis, angiogenesis, and osteogenesis properties has great clinical application potential as bone graft materials.