N-vinylformamide-grafted polypropylene (VFPP) was successfully synthesized through a free radical grafting reaction. Both polymeric methylene diphenyl diisocyanate (PMDI) and VFPP were effective compatibilizers for increasing both the strength and stiffness of the resulting wood-PP (polypropylene) composites. Both the modulus of rupture (MOR) and the modulus of elasticity (MOE) of the resulting wood-PP composites were further increased when PMDI and VFPP were used together as an integrated compatibilizer system. This new PMDI-VFPP compatibilizer system was comparable to maleic-anhydride-grafted polypropylene in terms of enhancing the strength and stiffness of the wood-PP composites. Study of the fractured surfaces of the wood-PP composites with scanning electron microscopy revealed that this new PMDI-VFPP compatibilizer system greatly improved the interfacial adhesion between wood and PP. This PMDI-VFPP compatibilizer system also greatly reduced the water absorption of the resulting wood-PP composites. In this PMDI-VFPP compatibilizer system, PMDI is proposed to function as a wood-binding domain and VFPP to function as a PP-binding domain. PMDI reacted with the amide group in VFPP, thus forming covalent linkages between PMDI and VFPP.