Ammonia (NH3) is a highly important industrial chemical used as fuel and fertilizer. The industrial synthesis of NH3relies heavily on the Haber–Bosch route, which accounts for roughly 1.2% of global annual CO2emissions. As an alternative route, the electrosynthesis of NH3from nitrate anion (NO3−) reduction (NO3−RR) has drawn increasing attention, since NO3−RR from wastewater to produce NH3can not only recycle waste into treasure but also alleviate the adverse effects of excessive NO3−contamination in the environment. This review presents contemporary views on the state of the art in electrocatalytic NO3−reduction over Cu-based nanostructured materials, discusses the merits of electrocatalytic performance, and summarizes current advances in the exploration of this technology using different strategies for nanostructured-material modification. The electrocatalytic mechanism of nitrate reduction is also reviewed here, especially with regard to copper-based catalysts.