Significance An ideal metal vascular stent has multiple properties for successful reendothelialization. These properties include 1) inhibiting thrombosis by preventing platelet activation/adhesion, 2) suppressing smooth muscle cell migration/proliferation, and 3) accelerating endothelial cell migration/proliferation. With an easy-to-perform, two-step surface bioengineering approach, the multifunctionalized stents reported here contain two vasoactive moieties (i.e., the nitric-oxide-generating organoselenium and the endothelial progenitor cell-targeting peptide) to satisfy all requirements. The surface engineering strategy presented here can be translated into clinical coatings for cardiovascular stents and will benefit enormously and globally the cardiovascular disease patients; it will, moreover, offer insights to engineering surfaces of blood-contacting devices.