Chemical grafting of salicylaldehyde onto the surface of carbon fibers (CFs) via the bridging 3‐aminopropyltriethoxysilane was reported to improve interfacial properties of composites. Surface microstructures, compositions, wettability, and surface energy of CFs before and after modification were studied. Single‐fiber tensile strength (TS) was also determined to evaluate the damage degree brought by using the grafting strategy to the fiber intrinsic strength. The interfacial shear strength of composites was characterized to confirm interfacial compatibility and adhesion between CFs and matrix resin. Antihydrothermal aging experiments were also carried out to evaluate their environmental stability. As a result, the introduced salicylaldehyde molecules could increase polar functional groups, roughness, and interfacial wettability of CFs, and thus enhance interfacial strength as well as the hydrothermal aging resistance of the resulting composites significantly. Such sharp improvements could be due to the increases of interfacial compatibility, mechanical interlocking, and chemical bonding at the interfacial region via the formation of salicylaldehyde‐modified interface. Meanwhile, the modification procedure does not decrease fiber TS.