CPC studies presented here provide a simple methodology for determining gallium in the mixed electrolyte medium of 4M NaClO4 + 0.5MNaSCN with a precision and accuracy of better than 0.5%, at milligram levels in presence of zinc as interfering element. To the best of our knowledge, this is the first report on controlled potential coulometric determination of gallium in synthetic Ga +U mixture solutions having varying concentration of gallium in the mixed electrolyte medium directly in the presence up to of 50% uranium and after separation of gallium in solutions having uranium above 50%. The insights gained in our study regarding the optimization of experimental parameters for the determination of gallium would provide guidelines for developing CPC methodology for the determination of gallium in gallium based semiconductor materials.