The rational design of non-noble metal-based electrocatalysts with efficient bifunctional catalytic activity is critical for the widespread application of zinc-air batteries (ZABs). In this study, an FeNi alloy encapsulated three-dimensional honeycomb-like network structure of carbon aerogels (FeNi/CAs) electrocatalyst was constructed using directional freeze-drying technology. The innovative architecture, combined with the synergistic effect between Fe and Ni, endows the FeNi/CAs catalyst with outstanding bifunctional catalytic activity compared with the introduction of a single metal in carbon aerogels. Specifically, the catalyst achieves a high half-wave potential (