We exploited an aqueous solution deposition technique to fabricate N-type ZnO and Al-doped ZnO (AZO) films with environmentally benign process at a very low temperature. ZnO, Zn, and Al were used in this study, instead of Zn(CH3COO)2, Al(NO3)3, and AlCl3 employed in previous investigations. Furthermore, the processing temperature was about 80°C which was lower than those of other fabrication techniques. The experimental results demonstrated that the resistivity of pristine ZnO and AZO films without any post-growth thermal annealing can be as low as ~2.0×10−2Ωcm and ~8.4×10−3Ωcm, respectively, and the transmittances were approximately 90% and 85%, respectively.