Particular aspects provide capacitors, and particularly ultracapacitors, comprising molecules suitable to substantially increasing 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, comprising at least three layers sealed in a fluid-tight covering, wherein a first layer comprises at least one electrolytic polymer molecule of positive charge and at least one nanoparticle; a second dielectric layer comprising at least one insulative polymer; a third layer comprising at least one electrolytic polymer molecule of negative charge and at least one nanoparticle. In certain aspects, the electrolytic polymer of the first layer comprises at least one high charge density polymer electrolyte of positive charge, and wherein the electrolytic polymer of the third layer comprises at least one high charge density polymer electrolyte of negative charge.