AbstractGreen ammonia synthesis through electrocatalytic nitrate reduction reaction (eNO3RR) can serve as an effective alternative to the traditional energy‐intensive Haber‐Bosch process. However, achieving high Faradaic efficiency (FE) at industrially relevant current density in neutral medium poses significant challenges in eNO3RR. Herein, with the guidance of theoretical calculation, we successfully designed and constructed a metallic CoNi‐terminated catalyst on copper foam, which achieves an ammonia FE of up to 100% under industrial‐level current density and very low overpotential (‐0.15 V versus RHE) in a neutral medium. Multiple characterization results have confirmed that the maintained metal atom‐terminated surface through interaction with copper atoms plays a crucial role in reducing overpotential and achieving high current density. By constructing a home‐made gas stripping and absorption device, we demonstrated the complete conversion process for high‐purity ammonium nitrate products, displaying the potential for practical application. Our work suggests a sustainable and promising process towards directly converting nitrate‐containing pollutant solutions into practical nitrogen fertilizers.This article is protected by copyright. All rights reserved