Electrochemical N 2 fixation is considered to be a promising alternative to Haber-Bosch technology. Inspired by the composition and structure of natural nitrogenase, Fe-doped VS 2 nanosheets were prepared via one-step solvothermal method. The electron transfer system mediated by organic conductive polymer (1-AAQ-PA) was constructed to promote the electron transfer between Fe-VS 2 nanosheets and the electrode in electrocatalytic N 2 reduction reaction (NRR). The obtained 1-AAQ-PAÀ Fe-VS 2 electrode converted N 2 to NH 3 with a yield of 31.6 μg h À 1 mg À 1 at À 0.35 V vs. reversible hydrogen electrode and high faradaic efficiency of 23.5 %. The introduction of Fe dopants favored N 2 adsorption and activation, while the LiÀ S bond between Fe-VS 2 and Li 2 SO 4 effectively inhibited hydrogen evolution. The highly efficient electron utilization in the electrocatalytic NRR process was realized using the 1-AAQ-PA as the electron transfer medium. Density functional theory calculations showed that N 2 was preferentially adsorbed on Fe and reduced to NH 3 via both distal and alternating mechanism.