A multilayer dielectric structure is formed by vacuum depositing two-dimensional matrices of nanoparticles embedded in polymer dielectric layers that are thicker than the effective diameter of the nanoparticles, so as to produce a void-free, structured, three-dimensional lattice of nanoparticles in a polymeric dielectric material. As a result of the continuous, repeated, and controlled deposition process, each two-dimensional matrix of nanoparticles consists of a layer of uniformly distributed particles embedded in polymer and separated from adjacent matrix layers by continuous polymer dielectric layers, thus forming a precise three-dimensional nanoparticle matrix defined by the size and density of the nanoparticles in each matrix layer and by the thickness of the polymer layers between them. The resulting structured nanodielectric exhibits very high values of dielectric constant as well as high dielectric strength.