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Nanocrystalline zinc-nickel alloy coatings were deposited from an alkaline zincate bath contained an organic additive that can reduce polarization and a complexing agent. SEM and TEM observations and XRD analysis were performed to examine the microstructure and phase composition of the coatings. The nickel content in deposits is 12.0~14.7% and the coating is consisted of single nanocrystalline γ-phase structure (Ni5Zn21), with grain average grain size about 15nm. The nanocrystalline zinc-nickel alloy coatings have better corrosion resistance, less brittleness and higher microhardness than the conventional zinc coatings.