Polymer blending is a method in which polymers with different properties are mixed so that each advantage appears in one polymer blend. Improved thermal and mechanical properties of blends can be prepared by blending with high-density polyethylene (HDPE) of a non-polar polymer and polyurethane (PU) of a polar polymer. However, a compatibilizer is required because it has the disadvantage that blending has low miscibility due to the different phases. In this study, HDPE/PU blends with new and excellent physical properties were developed through optimal composition with improved compatibility between the HDPE and PU. In addition, the effects of improving the physical properties through electron-beam crosslinking were confirmed. In general, a crosslinking structure of HDPE is formed by electron beam irradiation to increase its thermal stability and strength, but its elongation is rapidly decreased. In particular, the elongation of HDPE irradiated at 100 kGy was about 110%, which was decreased about five times compared to unirradiated HDPE (510%). However, the HDPE/PU blend with improved compatibility (PU 30) showed an elongation of about 450% while maintaining excellent strength (22.5 MPa), which was increased by about four times compared to the HDPE irradiated at 100 kGy. In particular, the thermal stability of PU 30 irradiated at 100 kGy at a high temperature (180 °C) was improved more than six times compared to the HDPE. Therefore, it is possible to develop HDPE/PU blends with new and excellent physical properties by improving compatibility and using electron beam crosslinking technology.