Particular aspects provide capacitors, and particularly ultracapacitors, including molecules suitable to substantially increase the capacitance of the capacitor, and methods for making same, Particular aspects provide ultracapacitors that include nanoparticles optionally coated with molecules, such as polymer electrolytes. Certain aspects provide an energy storage device or capacitor, including at least three layers sealed in a fluid-tight covering, wherein a first layer includes at least one electrolytic polymer molecule of positive charge and at least one nanoparticle; a second dielectric layer including at least one insulative polymer; a third layer including at least one electrolytic polymer molecule of negative charge and at least one nanoparticle. In certain aspects, the electrolytic polymer of the first layer includes at least one high charge density polymer electrolyte of positive charge, and wherein the electrolytic polymer of the third layer includes at least one high charge density polymer electrolyte of negative charge.