In this work, we have investigated the structure, morphology, photoluminescence, photocatalytic and photocurrent properties of ZnO thin films as a function of their film thickness (tZnO) fabricated via ultrasonic spray pyrolysis technique. The X-Ray diffraction patterns exhibited the formation of polycrystalline wurtzite phase of ZnO. Scanning electron microscopy images showed the uniform morphology with nanorod structure. The photosensitivity and photocatalytic efficiency are found to be optimum at tZnO = 1200 nm and are attributed to the improved photogeneration of charge carriers and higher concentration of oxygen vacancies. A direct correlation is established between the photosensitivity and photodegradation process. The incident photon-to-electron conversion efficiency (IPCE) and photocatalytic efficiency for the ZnO film at tZnO = 1200 nm are estimated to be 31.5% and 100% respectively. The obtained result suggests that ZnO thin films are potential candidates for applications in various optoelectronic devices.