Redox-active materials hold great promise as platforms for selective liquid-phase separations. In contrast to capacitive electrodes that rely purely on double-layer charge for deionization, redox-modified electrodes can be used to control Faradaic reactions at the interface to selectively bind various charged and uncharged molecules, thus modulating surface interactions through electrochemical potential solely. These electrodes can be composed of a range of functional materials, from organic and organometallic polymers to inorganic crystalline compounds, each relying on its own distinct ion-exchange process. Often, redox electrochemical systems can serve as pseudocapacitors or batteries, thus offering an advantageous combination of adsorption selectivity and energy storage/recovery. This review summarizes redox-interfaces for electrosorption and release, outlines methods for preparation and synthesis, discusses the diverse mechanisms for interaction, and gives a perspective on the future of redox-mediated separations.