The characteristics of a nickel sulfamate/iron chloride plating bath suitable for high rate electrodeposition of NiFe alloys are described. The effects of current density, electrolyte agitation, and Ni+2/Fe+2 content on deposit composition and plating current efficiency are explored via stripping voltammetry using a rotating ring-disk electrode. Specific plating bath formulations and operating conditions for depositing a wide range of alloy compositions at a variety of growth rates are illustrated. Special attention is given to determination of polarization and electrolyte mixing conditions for plating Permalloy and Invar. X-ray diffraction studies are used to investigate relationships between alloy composition and crystal structure. The implications for using the plating bath to electroplate composition-modulated alloys and 3D microstructures are discussed.