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Electrochemical reduction of nitrate to ammonia is of great interest in water treatment with regard to the conversion of contaminants to value-added products, which requires the development of advanced electrodes to achieve high selectivity, stability, and Faradaic efficiency (FE). Herein, nickel phthalocyanine was homogeneously doped into the fiber of a carbon nanotube (CNT) sponge, enabling the production of an electrode with high electrochemical double-layer capacitance (C DL) and a large electrochemically active surface area (ECSA). The as-prepared NiPc-CNT sponge could achieve 97.6% nitrate removal, 88.4% ammonia selectivity, and 86.8% FE at a nitrate concentration of 50 mg-N L–1 under an optimized potential of −1.2 V (vs Ag/AgCl). Meanwhile, the ammonia selectivity could be further improved at the high nitrate concentration. Density functional theory calculations showed that the exposure of Ni–N4 active sites could effectively suppress the hydrogen evolution reaction and dinitrogen generation, enhancing the ammonia selectivity and Faradaic efficiency. Overall, this work sheds light on the conversion of nitrate to ammonia on the metal phthalocyanine-based electrode, offering a novel strategy for managing nitrate in wastewater.