One nanostructured actuator embodiment includes an actuation region between electrical contacts. The actuation region includes an elastic matrix with embedded nanocomposite layered structures, which have inorganic material layers with pillared organic material structures between the inorganic material layers responsive to the surface acidity of the inorganic material layers. The elastic matrix allows transport of species for changing the surface acidity. A separator region is between the electrical contacts. A proton generation region capable of reversible electrochemical production and elimination of protons is provided, which may be a hydrogen storage material located on a side of the separator region opposite the actuation region, which may include metal hydride, or metal hydroxide. Alternatively, it may include an electrolytic solution and conductive particles within the elastic matrix for in situ electrochemical generation of an acid/base. The conductive particles may include carbon nanotubes, metal fibers, and/or metal nanoparticles. The nanocomposite structures may be generally aligned with a direction of work in the elastic matrix.