Electrocatalytic reduction of nitrate at noble metals is particularly sluggish at neutral pH, while nitrate reductase enzymes are highly active for selective reduction of nitrate to nitrite under these conditions. However,n oble metal electrodes can effectively reducen itrite, even at millimolar concentrations in neutralm edia. In this study,w ed emonstrate tandeme lectrochemicalr eductiono fn itrate to ammonia by combining Escherichia (E.) coli nitrate reductase (NarGHI) on an electrode with Pt or Rh nanoparticles. Under potentialc ontrol, the enzyme first reduces nitrate to nitrite, which is further reduced by the metal at as lightly more negative potential. This creates an ovel electrocatalytic relay cascade where the enzyme overcomes an inherentl imitation of the metal.T his proof-of-concept study,u sing biologicala nd metal catalysts supported on commercial carbon beads, demonstrates as imple approach to the assembly of 'hybrid' electrocatalysts.Anthropogenic imbalances in the global nitrogen cycleh ave raised increasing concern for their potentially noxiouse ffects on the environment and on public health.[1] Nitrate, being ap romoter of algal bloomsa nd ap recursort on itrite, at oxic anion, is the main target of international legislation setting am aximum allowable limit for its concentration in ground and drinking water.S ignificant quantities of nitrate from agricultural activities and acid rain reach groundwater,c alling for efficient approaches to wastewater remediation. Electrocatalytic methods stand poisedt ob ecomeaviable option, and electrochemicalr eactorsh ave been developed; [2] however,t here are significant barriers to their implementation. In particular, noble metal catalysts performp oorly in neutral media (the most commonp Ho fa griculture runoff) andr elease harmful products such as NH 2 OH. Bioelectrochemical reactorsa nd microbial fuel cells, [2,3] both of which incorporate bacterial cellsg rafted onto an electrode, have also been demonstrated for nitrater eduction. Selectivity to dinitrogen,t he mostd esirable product, is an issue fora ll availablen itrater eduction catalytic systems. [2b, 4] The two-electron reduction of NO À 3 to NO À 2 is the rate-determining step (Scheme 1) for noble metals, [2b] particularly at NO