Nitrate removal from groundwater remains a challenge. Here, we report on the development of a flow-through, electrically charged, granularactivated carbon (GAC)-filled column, which effectively removes nitrate. In this system, the GAC functioned as an anode, while a titanium sheet acted as a cathode. The high removal rate of nitrate was achieved through a combination of electrosorption and electrochemical transformation to N 2 . The column could be readily regenerated in situ by reversing the polarity of the applied potential. We demonstrate that in the presence of chloride, the mechanism responsible for the observed nitrate removal involves a combination of electroadsorption of nitrate to the anodically charged GAC, electroreduction of nitrate to ammonium, and the oxidation of ammonium to N 2 gas by reactive chlorine and other oxidative radicals (with nearly 100% N 2 selectivity). Given the ubiquitous presence of chloride in groundwater, this method represents a ready, green, and sustainable treatment process with significant potential for the remediation of contaminated groundwater.