Zn-30Al-xCu (x=0, 1, 2, 4) alloys were prepared by the spray atomization and deposition technique. The microstructures of the spray-deposited alloys were investigated by means of scanning electron microscope, transmission electron microscope, X-ray diffraction. The results indicate that the 1 wt. % Cu addition to spray-deposited Zn-30Al alloy does not make significant change in microstructure. However, with the 2, 4 wt. % Cu additions to the alloy, some ε-CuZn4 compounds with particle or irregular shapes were observed on the grain boundaries in the microstructures. Tensile test results confirmed that the 1 wt. % Cu addition displays superior tensile strengths, whereas the 2, 4 wt. % Cu additions led to the decreasing of the improvement effect of the tensile strengths.