Magnesium alloys have become the focus of attention as a new generation of vascular stent materials due to their excellent mechanical properties and degradability. However, their rapid degradation rate and poor surface endothelialization performance have become key factors limiting their clinical application. In this study, the Mg-Zn-Y-Nd (ZE21B) surface was modified with the magnesium fluoride (MgF2) corrosion-resistant layer, and the polydopamine (PDA) layer was used to immobilize the chitosan (CS)-ferulic acid (FA)/vanillic acid (VA) bioactive composite coating. The results of the electrochemical and hydrogen evolution experiments showed that the corrosion current density and hydrogen release of the modified ZE21B alloy significantly decreased, and its corrosion resistance was enhanced; the results of the hemolysis rate and whole blood experiments showed that the adhesion of blood components such as white blood cells and platelets on the surface of the modified ZE21B alloy significantly decreased, improving the blood compatibility of the magnesium alloy; the results of in vitro cell experiments showed that the modified ZE21B alloy effectively promoted endothelial cell (ECs) adhesion and proliferation, and inhibited smooth muscle cell (SMCs) pathological proliferation. These enhancements suggest that the CS-FA/VA coating significantly improves both the corrosion resistance and biological compatibility of the ZE21B alloy.