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As a high-active metal-free electrocatalyst for NH 3 production via NO reduction reaction, honeycomb carbon nanofiber achieves an NH 3 yield of 22.35 μmol h−1 cm−2 with a high Faradaic efficiency of 88.33%. [Display omitted] Electrocatalytic NO reduction is a promising technology for ambient NO removal with simultaneous production of highly value-added NH 3. Herein, we report that honeycomb carbon nanofiber coated on carbon paper acts as an efficient metal-free catalyst for ambient electroreduction of NO to NH 3. In 0.2 M Na 2 SO 4 solution, such catalyst achieves an NH 3 yield of 22.35 μmol h−1 cm−2 with a high Faradaic efficiency of up to 88.33%. Impressively, it also shows excellent stability for 10-h continuous electrolysis. Theoretical calculations reveal that the most active center of functional groups is –OH group for NO reduction with a low energy barrier (ΔG of 0.29 eV) for the potential-determining step (*NO + H → *HNO). [ABSTRACT FROM AUTHOR]