Abstract: The fabrication of one-dimensional metal/N-doped carbon materials has shown a promising prospect as efficient electrocatalysts for oxygen reduction reaction (ORR). Herein, CoNi alloy nanoparticles anchored on N-doped carbon nanotubes (CoNi@NCNT) are prepared by a dual-template strategy, using polypyrrole (PPy) tubes and CoNi-based metal-organic framework as the precursors. The as-formed CoNi@NCNT catalyst displays a half-wave potential (0.83 V) as well as good durability under alkaline medium. The excellent electrocatalytic performance is ascribed to a synergistic coupling of hierarchically tubular structure, highly electronic conductivity, and abundantly alloy-type active sites. When the CoNi@NCNT catalyst is applied in zinc-air battery (ZAB), the device displays a stable charge–discharge cycling performance. The present work affords a useful approach to constructing alloy/nitrogen-incorporated carbonaceous materials as bifunctional electrocatalysts for high-performance ZABs.