Electrocatalytic nitrogen reduction reaction (NRR) has attracted much attention as a sustainable ammonia production technology, but it needs further exploration due to its slow kinetics and the existence of competitive side reactions. In this research, xAu/MIL-101(Fe) catalysts were obtained by loading gold nanoparticles (Au NPs) onto MIL-101(Fe) using a one-step reduction strategy. Herein, MIL-101(Fe), with high specific surface area and strong N2 adsorption capacity, is used as a support to disperse Au NPs to increase the electrochemical active surface area. Au NPs, with a high NRR activity, is introduced as the active site to promote charge transfer and intermediate formation rates. More importantly, the strong interaction between Au NPs and MIL-101(Fe) enhances the electron transfer between Au NPs and MIL-101(Fe), thereby enhancing the activation of N2 and achieving efficient NRR. Among the prepared catalysts, 15%Au/MIL-101(Fe) has the highest NH3 yield of 46.37 μg h-1mg-1cat and a Faraday efficiency of 39.38 % at -0.4 V (vs. RHE). In-situ FTIR reveals that the NRR mechanism of 15%Au/MIL-101(Fe) follows the binding alternating pathway and also indicates that the interaction between Au NPs and MIL-101(Fe) strengthens the activation of the N≡N bond in the rate-limiting process, thereby accelerating the NRR process.