The development of new ecological materials to promote sustainability is being encouraged. Crosslinked biopolyethylene (BioPE)/noni flour (Morinda citrifolia) biocomposites were prepared using maleic anhydride-grafted polyethylene (PE-g-MA) and dicumyl peroxide (DCP). The biocomposites were processed in an internal mixer and injection molded. Torque rheometry, Izod impact strength, tensile strength, heat deflection temperature (HDT), differential scanning calorimetry (DSC), thermogravimetry (TG), and scanning electron microscopy (SEM) properties were investigated. Torque rheometry curves suggest that the biocomposites did crosslink due to the DCP attack on the BioPE chain. The BioPE/noni flour/PE-g-MA formulation with 0.5% and 1% DCP produced a higher level of crosslinking. As a result, the mechanical properties (impact strength, elastic modulus, and tensile strength) were improved. SEM showed fractured noni flour particles in the BioPE matrix with the formation of a tubular structure. The HDT increased, suggesting that the biocomposites exhibit enhanced thermomechanical strength. Furthermore, the biocomposites thermal properties obtained by DSC underwent few modifications. The TG results showed that the crosslinked biocomposites have better thermal stability than the noncrosslinked biocomposites. The crosslinking process of BioPE/noni flour biocomposites with the PE-g-MA/DCP hybrid is an effective way to improve the performance of these materials.