Metal–air batteries have attracted significant attention due to their excellent advantage of high-energy-density metal anodes with air cathodes. The development of structurally stable materials has been a great challenge for Zn-air batteries. Layered 2D materials provide unique opportunities due to their facial synthesis and structural stability. In this presentation, we demonstrate intercalated architecture TaSi₂N₄ layered material for cathode and anode of Zn–air batteries. The mechanistic aspects of Zn storage will be shown. These van der Waals materials undergo a phase during Zn loading. Interestingly, TaSi₂N₄ surface shows the two-electron mechanism of oxygen reduction. These layered materials will create new possibilities for the development of unique electrodes of Zn–air batteries.