Photoconduction mechanism of ZnO thin films that produced by Pulsed Electron Deposition method is systematically investigated by taking Transient Photocurrent Spectroscopy measurements for different atmospheres including high vacuum and air environments. Response and recovery rates of photocurrent in the air are faster than the rates in high vacuum condition. The results in the presented work clearly indicate that the photoconduction of ZnO thin films with high surface-area-to-volume ratio are surface-related and mostly governed by adsorption/desorption of oxygen and water molecules in the atmosphere. Therefore, the high surface interaction tendency of ZnO surface with the atmosphere inevitably leads to charge transfer from surface to adsorbates and/or vice versa.