Atomic layer deposition has been used to fabricate thin films of aluminum-doped ZnO by depositing interspersed layers of ZnO and Al 2O3 on borosilicate glass substrates. The growth characteristics of the films have been investigated through x-ray diffraction, x-ray reflection, and x-ray fluorescence measurements, and the efficacy of the Al doping has been evaluated through optical reflectivity and Seebeck coefficient measurements. The Al doping is found to affect the carrier density of ZnO up to a nominal Al dopant content of 5 at. %. At nominal Al doping levels of 10 at. % and higher, the structure of the films is found to be strongly affected by the Al 2O3 phase and no further carrier doping of ZnO is observed.