A significant challenge for energy storage technologies is to realize battery-level energy density and capacitor-level durability and power density in one device. By introducing an electrolyte composed of an anionic catholyte and a cationic anolyte into a symmetric carbon-based supercapacitor configuration, a hybrid electrochemical battery-supercapacitor system using soluble redox species delivers significantly improved energy density from 20 to 42 W.h/kg (based on the electrode mass) and stable capacities for > 104 cycles. The ionic species formed in the electrolyte are studied by UV-Vis, Raman and mass spectroscopy to probe the energy storage mechanism. The strategy is general and may provide a route to critically-needed fast-charging devices with both high energy density and power. © 2014 The Electrochemical Society.