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Surface immobilization of bioactive molecules has been a promising strategy to develop in situ endothelialization for cardiovascular implants. With the aim to construct endothelial cell specific coating with low fouling property, zwitterionic carboxybetaine methacrylate and butyl methacrylate were copolymerized as coating materials, spin‐coated onto substrates, and immobilized with endothelial cell selective peptide Arg‐Glu‐Asp‐Val (REDV) through functionalization of carboxy groups in carboxybetaine by NHS/EDC chemistry. Experimental results proved that carboxybetaine‐REDV coating maintained desirable antifouling ability and fine hemocompatibility. Separate culture and coculture of HUVECs (human umbilical vein endothelial cells) with HUASMCs (human umbilical artery smooth muscle cells) showed that the coating was able to enhance the competitive growth of endothelial cells while limiting the …