AbstractThe demand for epoxy (EP) in semiconductor, aerospace, and other applications is currently on the rise. However, pure epoxy is difficult to meet these requirements, such as low thermal conductivity and poor toughness. Therefore, in this paper, sulfonamides (SAs) and core‐shell silica (SLC‐SiO2) were grafted onto the surface of short carbon fibers (SCF) with sizes of 0.1–6 mm by the chemical grafting method. As a result, the surface activity of SCF was improved and the interfacial properties of the EP composites were enhanced. The interfacial compatibility of SCF grafted with SAs and SLC‐SiO2 in EP is greatly improved, resulting in stronger mechanical interlocking and chemical bonding ability between EP and SCF. The results showed that when the content of SCF@SAs@SLC‐SiO2/EP composites reached 0.3 wt% of SCF@SAs@SLC‐SiO2, the impact and tensile strengths were increased from 12.15 kJ·m−2 and 43.4 MPa to 16.93 kJ·m−2 and 74.97 MPa compared with the pure epoxy, which were improved 39.3% and 72.7%. In addition, the thermal conductivity of SCF@SAs@SLC‐SiO2/EP composites was also improved by 12.5% from 0.205 W·(m·K)−1 to 0.2306 W·(m·K)−1 compared with the pure EP. This is due to improved chemical interactions and mechanical interlocking at the fiber‐epoxy interface. This study provides a new method for the preparation of high‐performance SCF/EP composites.Highlights The amino group of sulfonamides was grafted with short carbon fiber to increase the surface active group of short carbon fiber. Sulfonamides react with carboxyl groups on the surface of core‐shell silica to form an “organic–inorganic” structure. Improve the surface roughness of short carbon fiber, and make it evenly dispersed in epoxy resin, so as to improve the performance of epoxy composite materials.