The enhancing effects of cross-linking by the addition of 1, 3, and 5 wt% of triallyl cyanurate (TAC) to blends containing 80 wt% of high-density polyethylene (HDPE) and 20 wt% of ethylene-propylene diene monomer (EPDM) during electron beam irradiation were investigated. More specifically, the thermal and mechanical properties were studied as a function of the electron beam irradiation dose and an amount of the cross-linking agent, such as triallyl cyanurate (TAC). The results showed that the values of the gel content, thermal stability, tensile properties, impact strength, and rheology increased with increasing irradiation dose up to 150 kGy. For higher doses, the values decreased. Addition of the cross-linking agent to the HDPE/EPDM blends showed an enhanced cross-linking effect of various properties during electron beam irradiation. The addition of 3 wt% of TAC led to the highest thermal and mechanical properties. An irradiation dose of 150 kGy with the addition of 3 wt% TAC was the optimal condition to obtain blends with the best properties.