Copper‐indium‐gallium‐selenium (Cu‐In‐Ga‐Se) precursor thin films have been prepared by electrodeposition techniques on molybdenum substrates. The films have been characterized by inductively coupled plasma spectrometry Auger electron spectroscopy, x‐ray diffraction, electron probe microanalysis, current‐voltage characteristics spectral response and electron‐beam‐induced current. Additional In or Cu, Ga, and Se have been added to the electrodeposited precursor film by physical evaporation to adjust the final composition to , and allowed to crystallize at 550°C A ZnO/CdS/ device fabricated using electrodeposited Cu‐In‐Ga‐Se precursor layers resulted in an efficiency of 12.3%.