We will describe the design principles by which naked nanocrystals (i.e. Those stripped of their native ligands) can be architectured into diverse 3-D mesoscale materials using block copolymers. Various polymer-architecturing paradigms will be discussed from a theor. perspective alongside exptl. results. Particular mention will be nanocrystal tethering domains that afford substantive enthalpic contribution to the free energy of co-assembly used to direct the nanocrystals into precision architectures at high vol. fractions. We will also show how those various architectures are useful in high-power energy storage applications.