Ammonia (NH 3 ) is a valuable chemical for fertilizer production and for use as an effective hydrogen carrier. Electrocatalytic nitrate reduction has recently received great attention as an alternative for NH 3 synthesis due to its kinetically favorable reaction. However, this promising strategy suffers from low Faradaic efficiency (FE) at large current density (>100 mA cm −2 ) and low nitrate concentrations because of the competing hydrogen evolution reaction. Herein, we report a catalyst consisting of earth-abundant cobalt−copper (Co 1−x Cu x ) nanoparticles supported on a three-dimensional substrate for efficient and selective NH 3 synthesis via electrocatalytic nitrate reduction. Typically, the optimized Co 0.5 Cu 0.5 catalyst performs at a high NH 3 Faradaic efficiency (FE) of over 95% at −0.03 V with NH 3 partial current density of ∼176 mA cm −2 at 50 mM nitrate, which is 7.3-and 1.7-fold higher than that of pure Co and Cu counterparts. Importantly, replacing Co with Cu enables the tuning of onset potential on Co catalyst maintaining high selectivity toward NH 3 . A stability test over 12 cycles confirmed the longterm operation of this catalyst. This work offers a facile strategy for tuning the catalyst's elemental composition to attain a desired electrocatalytic activity.