To create a new material with good biocompatibility and high mechanical strength for artificial organs, titanium (Ti) and segmented polyurethane (SPU) were bonded through 3-(trimethoxysilyl) propyl methacrylate (y-MPS), and specify causes governing the bonding strength of Ti/γ-MPS/SPU interface. The number of cross-links of SPU and the concentration of active hydroxyl groups on the surface oxide film of Ti were controlled by UV-irradaiton and hydrogen peroxide immersion. The number of cross-links of SPU was measured by differential scanning calorimetry (DSC) and the concentration of the active hydroxyl groups was also determined using a zinc-complex substitution technique. Consequently, Ti/y-MPS/SPU shear bonding stress was increased with the increase of the number of cross-links of SPU. In addition, the increase of cross-links in SPU also improved the Ti/y-MPS/SPU shear bonding stress.