Controlling the interface interaction of polymer/filler is essential for the fabrication of high-performance polymer composites. In this work, a core-shell structured hybrid (SiO(2)-GO) was prepared and introduced into an epoxy polymer matrix as a new filler. The incorporation of the hybrid optimized the modulus, strength and fracture toughness of the composites simultaneously. The ultrathin GO shells coated on silica surfaces were regarded as the main reason for the enhancement. Located at the silica-epoxy interface, GO served as an unconventional coupling agent of the silica filler, which effectively enhanced the interfacial interaction of the epoxy/SiO(2)-GO composites, and thus greatly improved the mechanical properties of the epoxy resin. We believe this new and effective approach that using GO as a novel fillers surface modifier may open a novel interface design strategy for developing high performance composites.