Nature Communications, Published online: 10 June 2026; doi:10.1038/s41467-026-74182-x Organonitrogen electrosynthesis restores N cycle sustainably but is limited by asynchronous proton-electron transfer. Here, the authors report a synergistic proton-electron donor interface of protonated polyaniline/graphite, enabling dual-path nitrate reduction for high efficiency oxime production.