In this paper, aluminum-doped zinc oxide (ZnO:Al or AZO) thin films are grown using atomic layer deposition (ALD) and the influence of postdeposition UV–ozone and thermal annealing treatments on the films’ properties are investigated. X-ray diffraction (XRD) revealed a polycrystalline wurtzite structure with a preferable (100) orientation. The crystal size increase after the thermal annealing is observed while UV–ozone exposure led to no significant change in crystallinity. The results of the X-ray photoelectron spectroscopy (XPS) analyses show that a higher amount of oxygen vacancies exists in the ZnO:Al after UV–ozone treatment, and that the ZnO:Al, after annealing, has a lower amount of oxygen vacancies. Important and practical applications of ZnO:Al (such as transparent conductive oxide layer) were found, and its electrical and optical properties demonstrate high tunability after postdeposition treatment, particularly after UV–Ozone exposure, offers a noninvasive and easy way to lower the sheet resistance values. At the same time, UV–Ozone treatment did not cause any significant changes to the polycrystalline structure, surface morphology, or optical properties of the AZO films.