We synthesized Al-doped ZnO (Al:ZnO) thin films by laser-assisted CVD and investigated their optical, electrical, and scintillation properties. The films exhibited a wurtzite-type ZnO structure with a strong (002) orientation. The averaged in-line transmittance in the visible wavelength region (380–780 nm) decreased from 90.4 to 49.0% as the Al concentration (CAl) increased from 0 to 35.8 at.%. The sheet resistance reached a minimum of 2.47 Ω/sq at CAl = 7.9 at.%. The Al:ZnO films with CAl = 2.7–7.9 at.% exhibited UV emission at 375 nm originating from free excitons, whereas films with higher CAl showed no obvious emission. The average decay time constant of the Al:ZnO film with CAl = 7.9 at.% was 2.10 ± 0.08 ns under 5.5 MeV α-ray excitation. Moderate Al addition improved electrical conductivity and photoluminescence intensity, whereas excessive Al led to the deterioration of these properties owing to the formation of an amorphous phase.