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Homogeneousd ispersion and ag ood interface between polymer and filler is crucial to obtain high-performance polymer composites. In this work, we use an ovel method employing organic aminopropyl-functionalized nanosilica sols (OAS-sols) to functionalize graphene oxide (GO) and thereby synthesize OAS covalently grafted graphene hybrid nanosheets (OAS-graphene). The spherical OAS covalently attached on the two-dimensional (2D) nanosheet GO surfaces creates OAS-graphene hybrids, which have large surface areas and homogeneous amino active sites distributed on the nanosheets. The OAS-graphene gave an improved dispersion and interface compatibility as well as ad ecreased thermali nterfacial resistance. As ar esult,t he thermalc onductivity and mechanical properties of the epoxy nanocomposites were significantly improved at low loading while maintaining high electricali nsulative properties.[a] Dr.