In this study, aminopropyl trimethoxysilane as an interfacial modifier was introduced on the surface of graphene (Gr) nanoplatelets. The effects of the silane‐modified graphene (SGr) loading (0, 0.05, 0.1, 0.3, and 0.5 wt %) and silane modification on the tensile, compressive, interlaminar shear stress (ILSS), and tribological properties of the epoxy‐based nanocomposites were investigated. Out of these specimens, the highest values of ILSS and compressive strength were related to the 0.3 wt % SGr–epoxy nanocomposite. The addition of SGr enhanced the tensile strength and strain to failure only at low contents (i.e., 0.05 wt %). Also, the tensile and compressive moduli were improved, and the highest values were observed at a 0.5 wt % SGr loading. In addition, decreases of approximately 40 and 68% in the coefficient of friction and wear rate, respectively, were observed at a 0.3 wt % SGr loading. Enhanced tensile, compressive, ILSS, and wear properties in the SGr–epoxy specimens were observed compared to those in the Gr–epoxy specimens. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019, 136, 47410.