Abstract In this study, the effects of silane‐treated nano‐CaCO 3 particles on the flexural, Mode‐I, Mode‐II and interlaminar shear strength (ILSS) properties of carbon fiber/epoxy composites are investigated experimentally. The surface of nano‐CaCO 3 particles is treated with a silane coupling agent, namely, (3‐Glycidyloxypropyl) trimethoxysilane (GPTMS). Three‐point bending, double cantilever beam (DCB), end‐notch flexure (ENF), and short beam shear (SBS) tests are carried out on the prepared composite specimens according to the relevant ASTM requirements. The results show that with the dispersion of 5 wt% silane‐treated nano‐CaCO 3 particles the flexural modulus, flexural strength, Mode‐I fracture toughness, Mode‐II fracture toughness, and ILSS values can be enhanced by 16.8%, 13.6%, 25.7%, 19.6%, and 19.8%, respectively, compared to reference composites. The storage modulus is also increased by about 15.3% with the silane‐treated nano‐CaCO 3 particles. The silane‐treated nano‐CaCO 3 particles had no significant effect on the glass transition temperature of the composites.