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In this work, we reported the synergistic effect of functional carbon nanotubes (CNTs) and graphene oxide (GO) on the anticorrosion performance of epoxy coating. For this purpose, the GO and CNTs were firstly modified by the 3aminophenoxyphthalonitrile to realize the nitrile functionalized graphene oxides (GO-CN) and carbon nanotubes (CNTs-CN). As modified GO-CN and CNTs-CN were characterized and confirmed by Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and gravimetric analyzer. It was found that about 19 and 24 wt% of 3-aminophenoxyphthalonitrile were grafted onto the surface of the GO and CNTs, respectively. The electrochemical impedance spectroscopy results showed that the GO-CN&CNTs-CN hybrid materials exhibit a remarkable superiority in enhancing the anticorrosion performance of epoxy coatings. Significant synergistic effect of the lamellar structural GO-CN and CNTs-CN on the anticorrosion performance of epoxy composite coatings was designed. Besides, the epoxy coating with 1 wt% of the GO-CN&CNTs-CN hybrid exhibited the best anticorrosion performance, in which the impedance showed the largest one (immersion in 3.5 wt% of NaCl solution for 168 hr).