<p>Anode alloying has been proven to be an effective solution to the self-corrosion problem of aluminum-air batteries in alkaline environments. However, the screening of such alloying elements currently relies mostly on traditional experimental methods, which are not only time-consuming but also costly. In this study, Density Functional Theory (DFT) calculations are employed to conduct element screening for the binary aluminum alloys used as anodes in aluminum-air batteries. By calculating the surface energy and work function of aluminum alloys, the corrosion resistance and electrochemical activity of the alloys are elucidated; meanwhile, the validity of the DFT calculation results is verified via self-corrosion tests, electrochemical tests, and full-cell tests. The results demonstrate that the screening principle for alloying elements is as follows: the doped alloying elements should enhance the corrosion resistance of aluminum alloys while ensuring favorable electrochemical performance; from the perspective of simulation calculations, this means that the doped elements should enable aluminum alloys to possess both favorable surface energy and work function. This study provides useful data support for the design of high-energy-efficiency anodes for aluminum-air batteries and aims to lay a foundation for the development of high-performance aluminum alloys for next-generation aluminum-air batteries.</p> Graphical Abstract <p></p>