Abstract: The interfacial shear strength (IFSS) between carbon fibers (CFs) and the matrix is crucial to the performance of CF-reinforced polymer composites. To evaluate the contribution of mechanical interlocking and chemical anchoring at the interfaces of a polyacrylonitrile-based CF (TORAYCA T800SC-12000-10E)-reinforced epoxy resin (EP: bisphenol A type epoxy resin and tetrafunctional epoxy resin) composites, the surface roughness and content of oxygen-containing functional groups of the CFs were respectively altered by ammonia treatment and electrochemical oxidation. The results showed that ammonia treatment increased the surface roughness without much change to the surface elemental composition, while electrochemical oxidation increased the number of surface oxygen groups without changing the surface roughness. The IFSS of CF/EP composites was tested by the micro-droplet method. The relationships between IFSS, and surface roughness and oxygen content were obtained by linear fitting. The results showed that in the interfacial bonding of CF to epoxy resin, the contribution of chemical anchoring to the IFSS is larger than that of mechanical interlocking.