In this study, high density polyethylene (HDPE) was combined with dicumyl peroxide (DCP) to produce crosslinked parts via rotational molding. The effect of DCP content (0.1–2.5 phr) on the crosslinking degree was investigated to determine its effect on the chemical, mechanical, physical, and thermal properties of HDPE. The gel content and crosslink density was found to increase with DCP content. These trends led to a reduction in the degree of crystallinity, melting, and crystallization temperature. Thermogravimetric analysis (TGA) showed that crosslinked HDPE (xHDPE) has higher thermal stability than the neat matrix in both air and nitrogen atmosphere. In addition, a direct relationship was observed between improved thermal resistance and higher impact strength. Finally, relationships between the tensile properties of xHDPE and the degree of crystallinity were observed, which were all controlled by the level of crosslinking. These results have the potential to advance the manufacturing of high performance materials suitable for a wide range of applications such as automotive parts, agricultural products, chemical storage tanks, large waste containers, and fuel tanks in general.