In this work, the effects of a heparin-functionalized coating on the growth behavior of vascular cells were studied. To retain its functionality, heparin was bound to a cationic plasma polymerized allylamine coating through electrostatic interaction. The heparin binding surface significantly inhibited human umbilical artery smooth muscle cell (HUASMC) adhesion and proliferation. In contrast, human umbilical vein endothelial cells (HUVECs) showed significant enhancement in cell adhesion, proliferation and migration, release of nitric oxide (NO) and secretion of prostaglandin I-2 (PGI(2)). The test of acute thrombogenicity assessed using human blood exhibited an excellent antithrombotic performance of the heparin grafted surface. The heparinized surface significantly promoted in vivo re-endothelialization and effectively inhibited thrombosis formation. These observations form an important framework for further deciphering the biological functions of heparin. It is highlighted that these striking findings may serve as a guide for the design of multifunctional vascular devices. Crown Copyright (C) 2012 Published by Elsevier Ltd. All rights reserved.