In this research, mercapto‐anchoring graphene oxide (GO) and epoxy‐anchoring SiO2 nanoparticles (NPs) were assembled by mercapto‐epoxy click chemistry to form three‐dimensional (3D) point‐plane structure nanomaterials (GO‐SiO2), and epoxy resin (EP) composites were prepared using the auxiliary thermal blending method. The relationships among surface interfacial interaction, dispersion, and mechanical properties of composites were systematically investigated. The Research finding shows that SiO2 NPs covalently bonding with GO increases interface compatibility and dispersion, which explains epoxy composite strengthening. Compared to epoxy resin, 0.1 wt% GO‐SiO2/EP composite has 38.65%, 36.15%, 44.64%, and 61.61% higher tensile strength, flexural strength, flexural modulus, and impact strengths. The enhancement mechanism of GO‐SiO2 toward EP was analyzed.