Electrocatalytic nitrogen reduction reaction (NRR) to produce ammonia as a promising technology for alternative Haber-Bosch process attracted vast attention. Unfortunately, the absorption of N2 and the breaking of stable triple bond still handicap the practical application of NRR. Here in our work, the Fe-doped Ni2P was fabricated and adopted as the advanced catalyst for NRR firstly. Benefited from the porous nanosheets structure, both the active sites and the surface area were increased. Meanwhile, along with the iron doping, the active centers on Ni site were activated and the new active centers on Fe site were created, thus promoting the adsorption of N2 and the weakening of NN bonds. Specifically, the Fe-Ni2P exhibited excellent activity, with NH3 yield of 88.51 μg h−1 mg−1cat. and FE of 7.92% being obtained at -0.3 V (vs. RHE), highlighting the heteroatom doping strategy as a novel guidance to the design of advanced NRR catalyst.