A process for forming nanostructures comprises generating charged nanoparticles with an electrospray system in a vacuum chamber and introduction of the charged nanoparticles to a region proximate to a charge pattern, so that the particles adhere to the charge pattern in order to form the feature. Two- or three-dimensional nanostructures may be formed by rapidly creating a charge pattern of nanoscale dimensions on a substrate using a normal electron beam or a microcolumn electron beam, generating high purity nanoscale or molecular size scale building blocks of a first type that image the charge pattern using the electrospray system, and then optionally sintering the building blocks to form the feature.