In this study, polypropylene random copolymer (PPR) composites were prepared by the addition of either three kinds of thermoplastic rubber (TPR) modifiers (types 2088A, 2095, and 2096) or an ethylene-octene copolymer (POE)/high-density polyethylene (HDPE; 2 :1 w/w) blend. Differential scanning calorimetry, wide-angle X-ray diffraction, and dynamic mechanical analysis were used to characterize the crystallization behaviors and dynamic mechanical properties of the PPR composites. The results indicated that PPR/POE/HDPE and PPR/TPR2088A had better comprehensive mechanical properties, especially the low-temperature toughness among all of the samples. The obtained PPR/POE/HDPE blends showed a high toughness and good stiffness in the temperature interval from 210 to 238C with the addition of only 10 wt % POE/HDPE. When the temperature continued to fall below 2108C, the PPR/TPR2088A composites exhibited a better impact toughness without a loss of too much stiffness. The good low-temperature toughness of those two composites was attributed to both the decrease in the crystallinity and the uniform dispersion, obvious interfacial adhesion, and cavitation ability of POE/HDPE and TPR2088A in the PPR matrix.