Carbon nanofiber (CNF)-reinforced polypropylene (CNF/PP) composites with different CNF contents were prepared by melt mixing, and the mechanical properties and crystallization behavior of the CNF/PP composites obtained were investigated. It was found that the tensile modulus of the composites was increased with the addition of CNFs, but their elongation at break and fracture strain energy were decreased, while the tensile strength of the composites was firstly increased and then decreased due to the agglomeration of CNFs at higher loading. Nonisothermal crystallization analysis showed that the CNFs played a role as nucleating agent in PP matrix, which led to increment in the crystallization rate and the degree of crystallinity of PP. Moreover, X-ray diffraction studies showed that the CNFs incorporated in the PP matrix favored the growth of (040)-oriented PP crystals. With the increase in the CNF content, the nucleating and orientation roles of the CNFs were obviously enhanced.