Magnesium is a biodegradable material that has potential application in cardiovascular stent development: its excellent mechanical properties and blood compatibility make it highly useful in interventional therapy. Nevertheless, the following shortcomings restrict its further application: antihyperplasia function and promoting surface endothelialization. In this study, we immobilized a specific link peptide of endothelial cells, Arg-Glu-Asp-Val (REDV), onto polydopamine (PDA)-deposited Mg–Zn–Y–Nd alloy surface via covalent reaction to improve the growth of the endothelial cells. The PDA/REDV coating with optimized parameters maintained the good blood compatibility of the Mg–Zn–Y–Nd alloy at the biomimetic speed of the blood flow and significantly inhibited the growth of the vascular smooth muscle cells and macrophage attachment/activation, which indicated its better functions in antihyperplasia and anti-inflammation. In particular, the PDA/REDV coating not only showed consistent results in promoting the attachment of endothelial cells as reported elsewhere, but also displayed the ability of enhancing the viability of endothelial cells (or inhibiting apoptosis), suggesting its pro-endothelialized function through different pathways. In summary, this PDA/REDV coating addressed the above-mentioned shortcomings of the magnesium alloy, which may promise its wider application.