To improve the biocompatibility of pulsatile ventricular assist devices (VADs), the blood-contacting surface of the segmented polyurethane (SPU) diaphragm employed in an electromechanical VAD was modified by introducing 2-methacryloyloxyethyl phosphorylcholine (MPC) units into its surface and forming an interpenetrating polymer network (IPN) structure, which contained independently cross-linked MPC polymer and SPU. The SPU diaphragm modified with an IPN structure was then assembled into a target test pump and underwent continuous pump operation at 37 degrees C for 2 weeks in a simulated systemic circulation using a mock circulatory loop. The surface characteristics of the pump diaphragm after 2 weeks of pump operation were then analyzed with an X-ray photoelectron spectroscope (XPS) and gold-colloid-labeled immunoassay. The XPS surface analysis of the IPN-modified SPU indicated the firm anchoring of MPC units even after 2 weeks of pump operation (the phosphor : carbon ratio was reduced by only 0.09%). The IPN-modified diaphragm prevented protein adsorption as well as cell adhesion in comparison to the unmodified SPU surface. This result thus validated that (1) the IPN structure could firmly secure MPC units to the SPU surface even in a high-mechanical-stress and high-shear environment, (2) the antithrombogenic power of MPC units remained unchanged after 2 weeks of continuous exposure to a high-shear environment, and (3) the IPN modified SPU cross-linked with MPC could be a powerful antithrombogenic surface for blood pumps used for chronic circulatory support of cardiac patients.