It is of significance to design catalysts for achieving high-performance electrochemical nitrate reduction to ammonia (NRA) in mild neutral media. However, the Faradaic efficiency and selectivity are still far from satisfaction. We present here the fabrication of an efficient catalyst by rationally doping Fe to Cu into a metasequoia-like nanocrystal of CuFe for NRA in neutral media. Fe doping is found to deepen energy level of Cu 3d band, favorably tuning adsorption energies of reaction intermediates to promote the NRA. At an applied potential of -0.7 V vs. RHE, the CuFe with ~2% Fe doping content delivers a catalytic current density of 55.6 mA cm -2 , which is 2.1 times as that of the Cu. The CuFe also exhibits a Faradaic efficiency up to 94.5%, and a good selectivity of 86.8%.