Abstract: The mechanical properties of carbon fiber (CF) reinforced cement-based materials were largely affected by the interfacial properties between CF and cement matrix. In this study, graphene oxide (GO) modified CF (GO/CF) was prepared by electrophoretic deposition of GO on the CF surface to strengthen its interfacial bonding with matrix. Firstly, after GO deposition, the physicochemical properties of CF surface are significantly enhanced. Secondly, the single fiber pullout test results show that the compared with the original CF, GO/CF has better interfacial bonding with the cement matrix, the average bond strength, friction bond strength and chemical debonding energy of GO/CF with the matrix are increased by 121%, 296% and 145.5%, respectively. On the one hand, the oxygen-containing functional groups of GO promote the formation of hydration products on the surface of CF, and the presence of oxygen-containing functional groups improves the inertness of CF surface, thereby improving the adhesion of CF to hydration products. On the other hand, the rough structure of GO increases the contact area between CF and hydration products. This ultimately provides excellent chemical adhesion and mechanical interlocking force between CF and cement matrix, thus improving the interface performance. Finally, the molecular dynamics simulation results show that GO on the CF surface can form stable ionic bonds and hydrogen bonds with calcium silicate hydrate (C-S-H). In addition, in the pull-out simulation, the maximum debonding force of CF in C-S-H/GO/CF is 200% higher than that in C-S-H/CF, because GO helps to transform the weak C-S-H/CF interface into one with stronger interfacial bonding at the C-S-H/GO and GO/CF interfaces. In summary, the addition of GO effectively improves the interfacial chemical bond interaction between CF and C-S-H, thus enhancing the interfacial bonding between the two.