The synergistic effect of ZnO and GO nanostructures on the surface modification of mild steel before the acrylic resin coating was studied. Firstly, the steel surface was pretreated in the presence of ultrasonic irradiation, and then ZnO nanostructures were synthesized by the cyclic voltammetry technique. GO nanosheets prepared by the modified hummer’s method were deposited on ZnO-containing surfaces using theelectrophoreticdepositio (EPD technique. GOcoatingswiththicknessesof2.84,4.47and9.42mmwere obtained by varying the EPD time, and the 4.47 mm was found as the optimum value for the fabrication of hybrid ZnO/GO structures. All samples were then covered with a thin layer of acrylic resin (10 mm) by the spin coating technique. The results indicated that the sample with underneath of hybrid ZnO/GO nanostructures shows significant improvement in anti-corrosion performance. In other words, Rp is increased from 150,000 V cm2 (in the rein coated sample) to 380,000 V cm2 (in the sample with hybrid nanostructures). The resulting surface has the potential to use as protective and glossy black coatings. The roleof underneathnature,surface roughness, and molecular interactions between oxygenfunctionalgroups of ZnO, GO, resin, and the metal in the enhanced corrosion protection was illustrated.