Electrochemical devices integrating a fuel cell with a hydrogen storage medium are able to function as secondary batteries. Batteries incorporating a partially oxygenated carbon anode with a RuO 2 /C cathode exhibit excellent reversibility, but their performance is not yet sufficient for secondary battery applications. This is due to excessive oxygenation of the anode, degradation of the cathode and the excess weight of the electrolyte membrane. In the present work, we addressed these challenges through various improvements in the design of a rechargeable proton-exchange membrane battery. These included coating the surface of a significantly oxygenated carbon anode (O/C atomic ratio 0.131) with carbon black nanoparticles, nanocrystallization of a carbon-free RuO 2 cathode (avg. crystallite size 1.1 nm) and the synthesis of an inorganic-organic composite electrolyte membrane. As a result of these optimizations, coulombic efficiencies of over 95% were achieved during charge/discharge over the voltage range of 0.0-1.5 V at 75 • C. The resulting device exhibited an initial capacity of 330 mAh g −1 and was stable over 300 cycles, with maximum energy and power densities of Hydrogen is a promising medium for the storage and supply of electricity through water-electrolysis/fuel-cell operation.1,2 The primary application of hydrogen in this context would be to store surplus power when the quantity of electricity produced by natural energy sources exceeds that required by a consumer.3-5 Rechargeable fuel cells capable of operating alternately in electrolyzer and fuel cell modes are recognized as the optimum systems because they are smaller and more compact than conventional systems based on isolated water electrolyzer and fuel cell units.6-8 The key technology necessary for such devices is hydrogen storage, which is currently accomplished via liquefaction and compression of the gas or by the physical or chemical adsorption of hydrogen atoms or molecules in/on materials such as metal or organic chemical hydrides.9,10 However, an energy input is required for these processes that in turn increases the overall cost. Furthermore, the hydrogen tanks and lines employed in such systems negatively impact their volumetric energy density.To mitigate these problems, rechargeable fuel-cell batteries (RFCBs) containing a hydrogen storage medium have been proposed. [11][12][13] During the operation of such batteries, hydrogen production, storage, supply and utilization processes must be conducted at the anode under the standard operational conditions of the cell, such as between room temperature and 80• C and at ambient pressure. In this context, oxygen-functionalized microporous carbons (MPCs) are promising hydrogen storage media, due to their excellent reversibility. 13 The redox pair between carbonyl (C=O) and phenol (C-OH) groups is one of the most important hydrogen carrier sites in such carbon anodes. The origin of this redox reaction is ascribed to the following equilibrium reaction between the two functional groups.This reaction...