Fluorine and aluminum co-doped ZnO (FAZO) films were deposited on glass substrates by RF magnetron sputtering. The effects of the substrate temperature (T-sub) on the structural, morphological, electrical, and optical properties of the films were investigated by X-ray diffraction analysis, atomic force microscopy, photoluminescence spectroscopy, Hall effect measurement, and ultraviolet-visible-near infrared spectrophotometry. All the thin films showed typical wurtzite structure with the c axis preferentially oriented perpendicular to the substrate. With increasing T-sub, the grain size shows a parabolic-like enhancement; the film surface became relatively smooth and dense, and the crystallinity was also improved. At T-sub = 320 degrees C, the films showed the best electrical properties, with a resistivity of 3.53 x 10(-4) Omega cm, Hall mobility of 39.33 cm(2)/V s, and carrier concentration of 4.50 x 10(20) cm(-3). An optical transmittance of more than 80% in a wide wavelength range from 400 to 1200 nm was also achieved. Perovskite solar cells employing the FAZO film had a higher power conversion efficiency than reference cells using F-doped SnO2 and Sn-doped In2O3, demonstrating its suitability for application in high-efficiency solar cells.