Blending is an effective method for improving polymer properties. However, the problem of phase separation often occurs due to incompatibility of homopolymers, which deteriorates the physical properties of polyblends. In this study, isotactic polypropylene was blended with lowdensity polyethylene. Crosslinking agent and copolymers of propylene and ethylene (either random copolymer or block copolymer) were added to improve the interfacial adhesion of PPI LDPE blends. The tensile strength, heat deflection temperature, and impact strength of these modified PP/PE blends were investigated. The microstructures of polyblends have been studied to interpret the mechanical behavior through dynamic viscoelasticity, wide-angle X-ray diffraction, differential scanning calorimetry, picnometry, and scanning electron microscopy. The properties of crosslinked PP/PE blends were determined by the content of crosslinking agent and processing method. For the material blended by roll, a 2% concentration of peroxide corresponded to a maximum tensile strength and minimum impact strength. However, the mechanical strength of those products blended by extrusion monotonously decreased with increasing peroxide content because of serious degradation. The interfacial adhesion of PP/ PE blends could be enhanced by adding random or block copolymer of propylene and ethylene, and the impact strength as well as ductility were greatly improved. Experimental data showed that the impact strength of PP/LDPE/random copolymer ternary blend could reach as high as 33.3 kg . cm/cm; however, its rigidity and tensile strength were inferior to those of PP/ LDPE/block copolymer blend.