Maleimidopropyltriethoxysilane grafted natural rubber (MISNR) was prepared by reaction of maleic anhydride grafted natural rubber and 3-aminopropyl triethoxysilane. MISNR was used as the compatibilizer of natural rubber/silica composites. The composites were prepared by two-step mixing procedures. The final mixtures were cured with optimum cure condition, which was established by a rheometer. Effects of the amounts of compatibilizer in the composites on the cure characteristics, morphology, thermal stability, and physical and mechanical behaviors were investigated. The composites having MISNR had shown cure characteristics and physical and mechanical properties superior to those without MISNR. Silica particles in the former appeared to be more uniform and reduced in size compared with the latter. The effects of the types of silica were also evaluated.