Abstract: Provided herein are multicomponent semiconductor films having a broad range of bandgaps and charge carrier characteristics. The semiconductor films include copper, zinc, tin, at least one substitutional metal and at least one chalcogen. Substitutional metals include those capable of substituting for a portion of copper, zinc, or both in the semiconductor films. Also disclosed are methods for making the films, including single-bath electrodeposition methods, and devices incorporating the films, including photovoltaic devices.