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Thin nanocrystalline transparent Al-doped ZnO (1–10 at.% Al) films were synthesized by solid-phase pyrolysis at 700 °C. Synthesized Al-doped ZnO films were investigated by X-ray diffraction (XRD), scanning and transmission electron microscopy (SEM, TEM). All obtained materials were crystallized into the wurtzite structure, which was confirmed by XRD. The material crystallinity decreases with the introduction of aluminum. SEM and TEM showed that the films are continuous and have a uniform distribution of nanoparticles with an average size of 15–20 nm. TEM confirmed the production of Al-doped ZnO films. The transmittance of Al-doped ZnO films in the range of 400–1000 nm is more than 94%. The introduction of 1% Al into ZnO leads to a narrowing of the band gap compared to ZnO to a minimum value of 3.26 eV and a sharp decrease in the response time to the radiation exposure with a wavelength of 400 nm. An increase in aluminum concentration leads to a slight increase in the band gap, which is associated with the Burstein–Moss effect. The minimum response time (8 s) was shown for film containing 10% Al, which is explained by the shortest average lifetime of charge carriers (4 s). [ABSTRACT FROM AUTHOR]