In this article, the graft copolymerization of methyl acrylate (M-A) onto nylon1010 by using potassium diperiodatonickelate(IV) [Ni(IV)]-nylon1010 redox system as initiator was studied in alkaline medium. The effect of different factors on grafting parameters was investigated. The structure of the graft copolymer was determined by infrared (IR), X-ray diffraction, and scanning electron microscope (SEM). It was found that Ni(IV)-nylon1010 system is an efficient redox initiator for this graft copolymerization. A single-electron transfer mechanism is proposed to explain the formation of radicals and the initiation. The graft copolymer was used as the compatibilizer in blends of poly(methyl methacrylate) (PMMA) and nylon1010. The SEM photographs indicate that the graft copolymer greatly improved the compatibility of the blend.