The process characteristics of the electrodeposition of nickel-chromium alloy from a trivalent chromium bath were investigated. Using an orthogonal design, the data from all the experiments in the set were taken together and analyzed to determine the effects of the various electrodeposition parameters. The chromium/nickel mole ratio, pH, rotation rate and temperature significantly affected alloy composition; the pH, chromium/nickel mole ratio, additive (formic acid) and temperature significantly affected current efficiency. Generally, the chromium/nickel mole ratio had a positive effect on the weight percentage of the chromium content in the deposit, but an adverse effect on alloy current efficiency. No monotonous dependence of alloy composition or current efficiency on the process parameters, including the current density, temperature, pH, rotation rate and additive agent, was observed. These novel results are discussed and explained. This study is a prelude to the development of a mechanistic model.