Abstract: The development of electrochemical energy storage technology represented by zinc-air batteries is one of the effective methods to solve the current energy and environmental problems. The key to zinc-air batteries lies in the development of low-cost, high-activity catalysts for the oxygen reduction reaction (ORR). Graphyne (GY) is widely used in the field of electrocatalysis due to its high specific surface area and unique electronic structure. In order to investigate the effect of nitrogen atoms on the electrocatalytic properties of graphyne, a novel nitrogen-doped graphyne (TCN-GY) is prepared by molecular design, with the specific introduction of cyano groups into graphyne for the first time using the Sonogashira coupling reaction.The effect of heat treatment on the structure of graphyne is investigated. Results show that certain heat treatment can regulate the pore structure of graphyne and expose the active sites, and the heat-treated nitrogen-doped graphyne derivative (TCN-GY-800) has high specific surface area as well as abundant nitrogen content. In the electrocatalytic oxygen reduction reaction tests, TCN-GY-800 shows high catalytic activity. It has a half-wave potential of 0.76 V, which is similar to that of commercial Pt/C catalysts (0.78 V). In zinc-air battery tests, the TCN-GY-800-based zinc-air battery boasts a maximum power density (142.9 mW/cm²) and specific capacity (570.0 mA·h/g), which are comparable to those of Pt/C-based zinc-air batteries. This indicates that the in situ doping strategy to prepare nitrogen-doped graphyne has a broad development potential in the field of ORR, which is expected to be further applied in energy- and environment-related applications.