Recent breakthroughs in particle synthesis leading to nanocolloidal particles of unusual shape and patterning have paved the way for a revolution in materials formed from the self-assembly of these building blocks. The unprecedented anisotropy of today's new nanoparticle and colloidal building blocks starkly contrasts with the isotropic, spherical colloids that have been the focus of particle assembly for more than a generation. No general theory exists to predict the range of structures possible for these new building blocks as a function of thermodynamic conditions, and the complementary problem of inverse design of a particular building block that can self-assemble into a desired target structure is difficult with as yet no standard design algorithm. In this talk, we present a conceptual framework with which to consider the key factors controlling the assembly of these new building blocks. We present results of computer simulations of patchy particle nanoparticle design and assembly, and show how various measures of anisotropy, including particle shape, patterning, functionalization and interaction selectivity, can be combined and exploited to achieve complex mesoscale one-, two- and three-dimensional structures such as wires, sheets, virus-like shells and colloidal “molecules”, diamond, icosahedral, gyroid, and other complex structures through self-assembly.