Functionalizing cardiovascular biomaterials with an extracellular matrix (ECM) via in vitro decellularization has been applied as an effective method to improve the biocompatibility of implants. However, the current ECM modified materials used for surface engineering implants have functional restrictions compared with the natural blood vessel due to distinguished cell phenotypes in vitro. Herein, we are inspired by the natural vascular basement membrane which is composed of an ECM secreted by physiological endothelial cells (EC) and smooth muscle cells (SMC), preparing a novel ECM coating by successive cell culture and decellularization: appropriately scaled hyaluronic acid (HA) micro-patterns are used to regulate the SMC phenotype to contraction and simulate the blood flow shear stress (BFSS) effect to control the EC physiological phenotype. The nature-inspired ECM coating significantly improves the material's hemocompatibility, cytocompatibility and tissue compatibility, and may be promising to break the function limitation of a single ECM and address more clinical complications.