The tuning of structural, optical, and electrical properties of Al-doped ZnO films deposited by atomic layer deposition technique is reported in this work. With the increasing Al doping level, the evolution from (002) to (100) diffraction peaks indicates the change in growth mode of ZnO films. Spectroscopic ellipsometry has been applied to study the thickness, optical constants, and band gap of AZO films. Due to the increasing carrier concentration after Al doping, a blue shift of band gap and absorption edge can be observed, which can be interpreted by Burstein-Moss effect. The carrier concentration and resistivity are found to vary significantly among different doping concentration, and the optimum value is also discussed. The modulations and improvements of properties are important for Al-doped ZnO films to apply as transparent conductor in various applications.Electronic supplementary materialThe online version of this article (doi:10.1186/s11671-016-1625-0) contains supplementary material, which is available to authorized users.