The graft copolymerization of 50/50 (w/w) styrene/methyl methacrylate mixtures onto natural rubber seed latex were carried out by using cumene hydroperoxide/sodium formaldehyde sulfoxylate dihydrate/EDTA-chelated Fe2+ as a redox initiator. The effects of the process factors such as the amount of initiator, emulsifier, and chain-transfer agent; monomer-to-rubber ratio; and temperature on the grafting efficiency (GE) and grafting level (GL) are reported. The mechanism of graft copolymerization was investigated. The synthesized graft copolymers were purified and then characterized by proton nuclear magnetic resonance (H-1-NMR) analysis. Transmission electron microscopy (TEM) was used to study the morphology of the graft copolymers. It appears that the formation of graft copolymers occurs on the surface of the latex particles through a chain-transfer process.