Porous yet densely packed carbon electrodes with high ion-accessible surface area and low ion transport resistance are crucial to the realization of high-density electrochemical capacitive energy storage but have proved to be very challenging to produce. Taking advantage of chemically converted graphene's intrinsic microcorrugated two-dimensional configuration and self-assembly behavior, we show that such materials can be readily formed by capillary compression of adaptive graphene gel films in the presence of a nonvolatile liquid electrolyte. This simple soft approach enables subnanometer scale integration of graphene sheets with electrolytes to form highly compact carbon electrodes with a continuous ion transport network. Electrochemical capacitors based on the resulting films can obtain volumetric energy densities approaching 60 watt-hours per liter.

A simple, bioinspired approach to effectively prevent the restacking of chemically converted graphene sheets in multilayered films is presented. The method enables the creation of a new generation of supercapacitors that combine high energy density, high power density, and high operation rates.

Modified graphene can self‐gel at the liquid–solid interface in a face‐to‐face manner to form an oriented conductive hydrogel film. This unusual gelation behavior enables a new generation of electroconductive hydrogels combining exceptional mechanical strength, high electrical conductivity, mechanical flexibility, and anisotropic responsive properties. Scale bar: 1 μm.