Zinc and Zn-Ni alloy compositionally modulated multilayer (CMM) coatings were electrodeposited on to a steel substrate by the successive deposition of zinc and Zn-Ni alloy sublayers from dual baths. The coated samples were evaluated in terms of the surface appearance, surface and cross-sectional morphologies, as well as corrosion resistance. The microstructural characteristics that were examined using the field emission gun scanning electron microscopy (FEGSEM) confirmed the layered structure, grain refinement of the zinc and Zn-Ni alloy CMM coatings, and revealed the existence of microcracks caused by the internal stress in the thick Zn-Ni alloy sublayers. The corrosion resistance that was evaluated by means of the salt spray test shows that the zinc and Zn-Ni alloy CMM coatings were more corrosion-resistant than the monolithic coatings of zinc or Zn-Ni alloy of the same thickness. The possible reasons for the better protective performance of Zn-Ni/Zn CMM coatings were given on the basis of the analysis on the micrographic features of zinc and Zn-Ni alloy CMM coatings after the corrosion test. A probable corrosion mechanism of zinc and Zn-Ni alloy CMM coatings was also proposed.