A novel nanoporous carbon/electrolyte hybrid material is reported for use in actuation. The nanoporous carbon matrix provides a 3D network that combines mechanical strength, light weight, and low cost with an extremely high surface area. In contrast to lower dimensional nanomaterials, the nanoporous carbon matrix can be prepared in the form of macroscopic monolithic samples that can be loaded in compression. The hybrid material is formed by infiltrating the free internal pore volume of the carbon with an electrolyte. Actuation is prompted by polarizing the internal interfaces via an applied electric bias. It is found that the strain amplitude is proportional to the Brunauer-Emmett-Teller (BET) mass specific surface area, with reversible volume strain amplitudes up to the exceptionally high value of 6.6%. The mass-specific strain energy density compares favorably to reported values for piezoceramics and for nanoporous metal actuators.