Zinc-nickel (Zn-Ni) alloys were electrodeposited in a noncyanide alkaline bath containing triethanolamine (TEA) and ethylenediamine (ED) as complexing agents for Ni2+ ions. The microstructure, surface morphology and alloy composition of the electrodeposited zinc-nickel alloys were investigated using X-ray diffraction (XRD), scanning electron microscopy (SEM) and X-ray fluorescence (XRF) analysis. A 2(3) full-factorial experimental design methodology was applied to identify the main and interaction effects of the variables, and the results were statistically analyzed. The results indicated that ED increased the particle size when the Ni additive concentration was 10 mL/L. When the Ni additive concentration was increased from 10 mL/L to 20 mL/L in the presence of 45 mL/L TEA, ED decreased the particle size and increased the smoothness and compactness of the alloy.