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Biodegradable magnesium‐based scaffolds present outstanding potential to revolutionize the treatment of coronary artery diseases, in which full recovery of arteries without long‐term irritation of implants is anticipated for averting adverse events associated with the permanent stents. However, overfast degradation of magnesium (Mg) alloys obstructs their extensive applications in terms of early structural failure and impaired biocompatibility. Herein, a facile copper‐incorporated coating system through nonaqueous phase synthesis of polydopamine is developed to facilitate Cu(II) capture along with robust film deposited on easily corrodible Mg, which subsequently enables sustained Cu(II) elution. It remarkably enhances corrosion resistance and impedes Mg degradation, which also contributes to improved, superior cytocompatibility, and abolished hemolysis. Moreover, through simultaneous control of Cu(II) and Mg(II) release to modulate the local microenvironment, a synergistic biochemical effect on desirable vascular cell selectivity is triggered for boosted endothelial cell viability and suppressed smooth muscle cell. Stent implantation into rabbit abdominal aorta thus exhibits accelerated re‐endothelialization completed in a week, and enhanced biological outcomes, alleviated complications and prolonged structural durability in 3‐month follow‐up. Collectively, this study opens up an alternative route of deploying a multifunctional surface modification strategy tailoring active interplay with the Mg matrix for better outcomes of next‐generation bioresorbable vascular stents. [ABSTRACT FROM AUTHOR]