Iron-nickel (Fe-Ni) plating bath solution chemistry was studied by determining the Fe-Ni equilibrium concentrations at various pH levels. It was found that the alloy composition is determined by solution equilibria, mass transfer of the electroactive species within the diffusion layer and by the surface coverage of the additives on the electrode. The effect of the rotation speed of the disc electrode and the presence of organic additives on the deposition of Fe-Ni alloys are evaluated. Boric acid increases the absolute iron deposition rate, while it inhibits the rate of nickel reduction. Saccharin and ethylene diamine influence the metal deposition rate but are not as effective as boric acid.