Single-bath electrodeposition of polycrystalline thin films for photovoltaic applications is described. was deposited onto Mo electrodes from low concentration aqueous baths containing , , , and . Buffering the solutions to stabilized bath chemistry and improved film composition. Bath concentrations were shown to affect composition of deposited films, with a bath ratio of 1.75 required to maintain suitable deposited Se and Cu levels, while could be adjusted to control deposited In and Ga. Deposited films initially exhibited significant cracking, which was prevented by lowering the in the bath, and contained as secondary phases, resembling cauliflower florets, embedded in the film surfaces. The formation of these secondary phases was overcome by pretreating the Mo electrodes with a short deposition from the bath. This, coupled with a multipotential deposition regime, led to growth of smooth, compact, crack-free films of near stoichiometric values. Mechanisms of film growth and morphology control are discussed. All as-deposited films exhibit low crystallinity, and for device processing require recrystallization by annealing in an atmosphere. Promising preliminary results of electrodeposited devices are presented.