In order to improve the hemocompatibility of polycarbonateurethane (PCU), the biomimetic phosphorylcholine (PC) group was introduced onto material surface. Brush structure having PC groups was formed by ultraviolet (UV) initiated polymerization of 2-methacryloyloxyethyl phosphorylcholine (MPC) to improve the hydrophilicity and hemocompatibility of PCU surfaces. Fourier transform infrared (FTIR), X-ray photoelectron spectroscopy (XPS), scanning electrical microscopy (SEM) and water contact angle were used to characterize the chemical and physical properties of the modified PCU surfaces. Compared with original PCU, the PC-grafted PCU surfaces showed significantly high hydrophilicity as indicating by low water contact angle. The hemocompatibility of the PC-grafted PCU surfaces was evaluated by platelet adhesion test. The PCU surfaces modified with phosphorylcholine zwitterionic brushes showed effective resistance to platelet adhesion and high hemocompatibility. These PC-grafted PCU materials will have potential application as blood-contacting materials or devices due to their good mechanical and hemocompatible properties.