Accelerated industrialization disrupts the global nitrogen cycle, resulting in alarmingly increased nitrate in groundwater and other water bodies. Electrocatalytic nitrate reduction (NO3RR) with high automation can effectively remove nitrate from polluted water, thus avoiding nitrate accumulation. However, the sluggish cathode reaction kinetics severely hampered the efficiency of NO3RR. Developing high-performance cathode catalysts is of great significance for boosting NO3RR. Compared with pure metal catalysts, bimetal catalysts can further improve the cathode activity and selectivity to nitrogen or ammonia in the electrocatalytic process, attracting extensive research interest. In this review, we discussed the background of denitrification requirements and the development status of bimetallic denitrification catalyst. Metallic cathode catalysts, such as noble-metal, 3d transition metal, main group metal, are described emphatically. Finally, present challenges and future outlook on bimetallic denitrification catalysts are depicted.