Surface modification of biomaterials for rapid endothelialization is a promising approach for improving long-term patency of artificial vascular grafts (e.g. polytetrafluoroethylene, PTFE) with small-caliber vascular (<6 mm). However, surfaces modified with traditional strategies using hydrophilic polymers may be excessively hydrophilic to limit endothelial cell adhesion and formation of confluent endothelial lining. In this study, a triblock functional protein cofp-MZY/R was fabricated with cell selectivity of endothelial cells (ECs) over smooth muscle cells (SMCs) for endothelialization on PTFE. This rational designed triblock protein consisted of mussel-inspired domain, zwitterionic polypeptide and bioactive peptides (YIGSR and REDV), in which Dopa was efficiently obtained with residue-specificity in vivo. The triblock protein could facilely form coating on PTFE surface and the resulting protein coating exhibited moderate nonspecific resistance of protein and platelets. Together with bioactive peptides tail, it was available for cell attachment on surfaces. As protein material, this coating displayed remarkable biocompatibility through cytotoxicity and hemolysis measurements. Moreover, cellular behavior assay demonstrated that triblock protein coating could selectively promote adhesion, proliferation and migration of ECs rather than SMCs. This mussel-inspired triblock functional protein coating indicated a promising strategy for endothelialization of artificial vascular grafts. (C) 2020 Elsevier Inc. All rights reserved.