The organ-on-a-chip model mimics the structural and functional features of human tissues or organs and has great importance in translational research. For vessel-on-a-chip model, conventional fabrication techniques are unable to efficiently imitate the intimal-medial unit of the vessel wall. Bioprinting technology, which can precisely control the organization of cells, biomolecules, and the extracellular matrix, has the potential to fabricate three-dimensional (3D) tissue constructs with spatial heterogeneity. In this study, we applied the gelatin-methacryloyl-based bioprinting technology to print 3D construct containing endothelial cells (ECs) and smooth muscle cells (SMCs) on a microfluidic chip. Compared with traditional culture system, EC-SMC coculturing chip model upregulated αSMA and SM22 protein expression of the SMC to a greater degree and maintains the contractile phenotype of the SMC, which mimics the natural vascular microenvironment. This strategy enabled us to establish an in vitro vascular model for studies of the physiologic and pathologic process in vascular wall.