Methods for assemblies of anisotropic nanoparticles which includes forming a substantially close packed dense layer by assembling a plurality of anisotropic nanoparticles, each of the plurality of anisotropic nanoparticles having a) a first dimension that is substantially different than both a second dimension and a third dimension and b) a non-random nanoparticle crystallographic orientation that is substantially aligned with the first direction, wherein assembling includes mechanically interacting the plurality of anisotropic nanoparticles by imposing a delocalized force that defines a direction that is substantially perpendicular to a basal plane of the substantially closed packed dense layer; and imposing a fluctuating force to which the anisotropic nanoparticles respond, which is sufficient to overcome a short range weak attractive force between members of the plurality of anisotropic nanoparticles with respect to anisotropic nanoparticles that are not substantially overlapping.