This letter describes the heteroepitaxy of InP on Si by MOCVD. A new epitaxial structure with a thin GaAs intermediate layer (InP/GaAs/Si) is proposed to alleviate the large lattice mismatch (8.4%) between InP and Si. Using this structure, a 4-inch InP single crystal with a mirror-like surface and good thickness uniformity (Δd/d=±10%) was obtained. Residual stress in the InP film was 5.7±108 dyn/ cm2 for the InP/GaAs/Si structure, as compared to 8.3×108 dyn/cm2 for the InP directly grown on Si. This shows that the GaAs intermediate layer is also effective in reducing the residual stress in the InP epilayer.