AbstractElectrochemically reducing nitrate (NO₃⁻), a common water pollutant, to valuable ammonia (NH₃) offers a green, sustainable, and decentralized route for ammonia synthesis. Electrochemical nitrate reduction reaction (NO₃⁻RR) involves two crucial reaction steps: nitrate deoxygenation followed by nitrite hydrogenation; in particular, the nitrite hydrogenation reaction is the rate‐determining step (RDS) for NO₃⁻RR. In this work, an atomically dispersed cobalt‐phosphorus (Co─P) catalytic pair (CP) with strong electronic coupling is reported. The Co site in Co─P CP effectively activates NO₃⁻, while the P site in Co─P CP facilitates water dissociation to release H⁺, synergistically enhancing the thermodynamic and kinetic performance of electrochemical nitrate reduction to ammonia.