Al-doped ZnO (AZO) thin films with various Al concentrations were synthesized on Si(001) substrates with native oxide layers by atomic layer deposition process. The effects of the Al concentration on the microstructural characteristics of the AZO thin films grown at 250 degrees C and the correlation between their microstructural characteristics and electrical properties of the AZO thin films were investigated by AFM, XRD, HRTEM and Hall measurements. The XRD and HRTEM results revealed that the crystallinity and electrical properties of the undoped ZnO thin films were enhanced by 2.48 at% Al doping. However, 12.62 at% Al doping induced the deterioration of their crystallinity and electrical properties due to the formation of nano-sized metallic Al clusters and randomly oriented ZnO-based nano-crystals. To enhance the electrical properties of the AZO thin films while maintaining their crystallinity and electrical properties, a moderate Al concentration has to be chosen under the solubility limit of Al in ZnO.