InP layers grown on Si (001) were achieved by the two-step growth method using gas source molecular beam epitaxy. The effects of growth temperature of nucleation layer on InP/Si epitaxial growth were investigated systematically. Cross-section morphology, surface morphology and crystal quality were characterized by scanning electron microscope images, atomic force microscopy images, high-resolution X-ray diffraction (XRD), rocking curves and reciprocal space maps. The InP/Si interface and surface became smoother and the XRD peak intensity was stronger with the nucleation layer grown at 350 °C. The Results show that the growth temperature of InP nucleation layer can significantly affect the growth process of InP film, and the optimal temperature of InP nucleation layer is required to realize a high-quality wafer-level InP layers on Si (001).