The latex mixing is the most commonly used method for preparation of graphene and graphene derivatives/rubber nanocomposites. In this paper, on the basis of latex mixing method, the technology of electrostatic self-assembly was applied to preparation of graphene based/rubber nanocomposites. The positively charged cetyltrimethylammonium bromide modified mesoporous silica(MCM-NH₄H), the negatively charged graphene oxide, and the negatively charged rubber latex particles were blended in an aqueous solution, and a new type of nanocomposite was formed by electrostatic self-assembly. The structures of the prepared nanocomposites were characterized by IR, XRD and SEM. The effects of GO and MCM-NH₄H on the properties of the nanocomposites were systematically studied. The results show that the synergy between MCM-NH₄F and GO greatly improves the performances of the nanocomposites. When the content of GO is 0.75 phr, the tensile strength of the composite reaches 29.4 MPa, which is 32.6% higher than that of the material without GO. In addition, the dielectric properties of the material are also improved.