Fluorine- and aluminum-codoped ZnO (FAZO) thin films are sputtered on Corning glass substrates using an RF magnetron sputtering system. The structural, electrical, and optical properties of the deposited thin films are investigated under the as-sputtered condition and after annealing at temperatures of 200–400 °C. X-ray diffraction (XRD) analysis results show that a higher annealing temperature is beneficial in improving the crystallinity of the FAZO films. An annealing temperature of 400 °C results in the lowest electrical resistivity (4.1 × 10−4 Ω·cm) and highest average transmittance (78.43%) among the deposited films. Moreover, an annealing temperature of 400 °C increases the energy bandgap from 3.06 eV under the as-sputtered condition to 3.21 eV after annealing and promotes a strong grain growth effect. As a result, the annealed FAZO film is an ideal material for solar cells and photosensor applications.