This paper describes the effect of Al doping (0 at.% to 6 at.%) on the structural and optoelectronic properties of nanocrystalline ZnO thin films deposited by thermal evaporation. X-ray diffraction patterns confirm that an increase in Al concentration (from 0% to 6%) in ZnO lowers the crystallinity of the films and reduces grain size. Al doping is also found to influence the optical properties of the ZnO thin films. Visible transmittance above 85% was obtained by increasing the Al doping to 6%. The optical bandgap was found to vary from 3.20 eV to 3.97 eV with changing Al content from 0% to 6%, which is in accordance with the Burstein-Moss shift. The mobility of ZnO thin films can be varied from 5.60 cm 2 /Vs to 24.25 cm 2 /Vs, the carrier concentration from 5.93 9 10 18 /cm 3 to 9.11 9 10 20 /cm 3 , and the resistivity from 4.62 9 10 Ă4 X cm to 4.34 9 10 Ă2 X cm, depending on the Al doping concentration (0% to 6%). This study suggests that ZnO:Al films can be tailor-made to meet the requirements for various optoelectronic applications such as flexible photocells or ultraviolet (UV) photodetectors covering a wide range of short wavelengths.