A silane coupling agent was used to modify the surface of expanded graphite (EG), which was subsequently used as a thermally conductive filler to fabricate diglycidylether of bisphenol-A (DGEBA)/EG composites with high thermal conductivity via hot blending and compression-curing processes. The surface characteristics of silane coupling agent-modified EG (Si@EG) were characterized by a variety of analytical techniques. The effects of the Si@EG content on the thermal conductivity, thermal stability, impact strength, and morphology of the DGEBA/Si@EG composites were investigated. The results revealed that the addition of 80 wt.% Si@EG increased the thermal conductivity of the composites from 0.17 to 10.56 W/m K, which was 61.1 times higher than that of pristine DGEBA. The initial decomposition temperature of the composite containing 80 wt.% Si@EG was 60.6 C higher than that of pristine DGEBA. The impact strength of the composites decreased from 2.0 to 0.87 kJ/m 2 when the Si@EG content increased from 0 to 80 wt.%. The scanning electron microscopy images of the fractured surfaces revealed that the EG sheets in the DGEBA matrix formed a continuous thermally conductive path at high Si@EG contents.