The effect of reactive gases - oxygen and hydrogen - on the tunable work function of Al-doped ZnO (AZO) films was studied. An increase in the work function with an increase in the oxygen flow rate was mainly interpreted as reflecting a decrease in the carrier concentration, which was attributed to the filling of oxygen vacancies. However, a decrease in the carrier concentration would result in the resistivity increasing sharply. This article presents a new concept for improving the performance of organic light-emitting diodes (OLEDs) through easy and effective hole injection from a multilayer AZO anode to the organic layer. A bilayer AZO film prepared using a tunable work function technique was used to modify the surface of AZO anodes and to ensure that the anodes had low resistivity. The AZO anode stacked with high-work-function AZO films, similar to hole transport buffer layers, had a low turn-on voltage of 2.89 V, and its luminance efficiency and power efficiency were 5.01% and 6.1% greater than those of tin-doped indium oxide anodes used in OLEDs.