Interfacial properties play a critical role in the performance of carbon fiber-reinforced composites (CFRPs). However, poor interfacial interactions between carbon fiber (CF) and polymer matrix often limit the performance improvement of CFRPs. In the present work, ethylenediamine functionalized graphene oxide (FGO) and oxidized-carbon fiber (oxidized-CF) are applied to prepare CFRPs through electrostatic self-assembly. Results of Raman, TGA, SEM, and dynamic contact angle analyses confirm that FGO nanosheets are tightly bonded onto the oxidized-CF surface. DMA results show a small increase of T g of the oxidized-CF-FGO composites, as well as a great increment of energy storage modulus (E') compared to that of the untreated CF composites, which indicates an enhancement of interfacial properties. More importantly, the interfacial shear strength shows a great improvement of 30.4%, reaching 58.7 MPa. The interfacial enhancement mechanisms are further discussed based on the microstructure and performance evaluation results.