Li-incorporated ZnO thin films were deposited by using ultrasonic-assisted spray pyrolysis deposition (SPD) system. To investigate the effect of Li-incorporation on the performance of ZnO thin films, the structural, electrical, and optical properites of the ZnO thin films were analyzed by means of X-ray diffraction (XRD), field-emssion scanning electron microscopy (FE-SEM), Hall effect measurement, and UV-Vis spectrophotometry with variation of the Li concentraion in the ZnO sources. Without incorporation of Li element, the ZnO surface showed large spiral domains. As the Li content increases, the size of spiral domains decreased gradually, and finally formed mixed small grain and one-dimensional nanorod-like structures on the surface. This morphological evolution was explained based on an anti-surfactant effect of Li atoms on the ZnO growth surface. In addition, the Li-incorporation changed the optical and electrical properties of the ZnO thin films by modifying the crystalline defect structures by doping effects.