The effect of dicumyl peroxide (DCP) content on the gel fraction, mechanical, dynamic mechanical, and thermal properties of linear low-density polyethylene (LLDPE)/ethylene-co-methyl acrylate (EMA) blends were studied. Gel content of the blends increases with increasing DCP content, and EMA is more prone to crosslinking than LLDPE. Wide-angle X-ray diffraction (WAXD) and differential scanning calorimetry (DSC) were used to study the effect of DCP crosslinking on percent crystallinity and crystalline structure of the blends and individual components. At lower level of DCP loading, crosslinking process does not have significant effect on the crystalline structure of the LLDPE, which was confirmed from the percent crystallinity and lattice distance value. However, at higher DCP content, percent crystallinity decreases significantly.At lower EMA concentration (<50%), percent crystallinity and lattice distance remain unchanged up to 2 wt % of DCP. For EMA contents of more than 50 wt %, increasing DCP content reduces the crystallinity of the blends and increases the lattice distance. The highest level of mechanical and dynamic mechanical properties was observed for 60/40 LLDPE/EMA blends at 2 wt % DCP. Addition of LLDPE-g-MA (3 wt %) as a compatibilizer enhances the properties of the vulcanizates. Blends crosslinked with DCP up to 0.3 wt % can easily be reprocessed.