AbstractGa and Al doped ZnO thin film electrodes are spray deposited and explored for photocatalytic deterioration of methylene blue dye. X‐ray diffraction unveils both films to have highly textured growth along the (002) plane. The surface morphology is found to have near spherical and distorted rectangular particles for Ga and Al dopants, respectively. Photoluminescence emission study reveals that both films have visible light emissions in the violet, blue, and green regions due to oxygen vacancy defects. The deposited films exhibit a reasonably higher transmittance of 89 and 77 % with mobility of 30.5 and 29.6 cm2/Vs for Ga and Al doped ZnO, respectively. Cyclic test and photo‐corrosion studies performed for selected samples were indicating significant stability. Based on these findings the electrodes are explored for the photocatalytic degradation of methylene blue dye and are found to have significant efficiency upon LED and sunlight irradiation.