A study reports the development of spin-polarized Fe₁-Ti pairs on a monolithic titanium electrode, which significantly enhances the electroreduction of nitrate to ammonia (NITRR). By manipulating oxygen vacancies, the researchers achieved a high ammonia yield rate of 272,000 µg h⁻¹ mg⁻¹Fe and a Faradaic efficiency of 95.2% at -0.4 V vs. RHE, surpassing conventional electrocatalysts. The spin-polarized Fe and Ti atoms facilitate the deoxygenation of nitrate and hydrogenation of *NO, improving NITRR efficiency. The study also demonstrates the integration of a flow-through electrolyzer with a membrane-based ammonia recovery unit, enabling efficient nitrate conversion and in-situ ammonia recovery. The spin-polarized Fe₁-Ti pairs show excellent stability and performance, offering a promising strategy for nitrogen wastewater treatment and ammonia production. The findings highlight the importance of spin polarization in enhancing electrocatalytic reactions and provide a new approach for designing advanced electrocatalysts.A study reports the development of spin-polarized Fe₁-Ti pairs on a monolithic titanium electrode, which significantly enhances the electroreduction of nitrate to ammonia (NITRR). By manipulating oxygen vacancies, the researchers achieved a high ammonia yield rate of 272,000 µg h⁻¹ mg⁻¹Fe and a Faradaic efficiency of 95.2% at -0.4 V vs. RHE, surpassing conventional electrocatalysts. The spin-polarized Fe and Ti atoms facilitate the deoxygenation of nitrate and hydrogenation of *NO, improving NITRR efficiency. The study also demonstrates the integration of a flow-through electrolyzer with a membrane-based ammonia recovery unit, enabling efficient nitrate conversion and in-situ ammonia recovery. The spin-polarized Fe₁-Ti pairs show excellent stability and performance, offering a promising strategy for nitrogen wastewater treatment and ammonia production. The findings highlight the importance of spin polarization in enhancing electrocatalytic reactions and provide a new approach for designing advanced electrocatalysts.