In this paper, the electrodeposition process of Cu-Zn alloy powders from pyrophosphate-based electrolytes was investigated as a function of deposition parameters under direct current. The effects of deposition parameters such as current density, electrolyte composition (Cu/Zn mole ratio), mechanical stirring speed, and temperature on the Cu content of alloy powder and cathodic current efficiency were evaluated using the response surface methodology. The empirical models developed in terms of deposition parameters have been found statistically adequate to describe the process responses. The study revealed that as far as the copper content was concerned in the alloyed powders; all parameters selected have positive correlations. However, high stirring speed and low current density lead a greater current efficiency. The morphology and chemical composition of the electrodeposited Cu-Zn alloy powders were investigated using SEM, EDS, and ICP analysis. SEM analysis showed that the powder morphology is considerably affected by the cathodic current density and stirring speed.