Rare-earth nanocrystals (RE NCs) bring the distinct optical, magnetic, and catalytic properties of bulk rare-earth materials to a solution-processable and biorelevant size-regime. The chemistry of the rare-earth elements also enables the bottom-up synthesis of monodisperse anisotropic NCs with distinct morphologies. Herein, I present the synthesis of four anisotropic rare-earth nanocrystalline systems, namely dysprosium fluoride nanoplatelets, 90Y-doped sodium yttrium fluoride nanophosphors, etched sodium yttrium fluoride nanohourglasses, and ceria-coated palladium nanoflowers, that were elucidated through the use of a semi-combinatorial approach for parallel solvothermal synthesis that was developed over the course of these studies. Methodology for elementally mapping these nano-heterostructures using transmission electron microscopy are also described herein. These systems reveal mechanisms by which the ligand environment and surface treatments can affect the growth of nanocrystalline materials, as well as how these bottom-up approaches can lead to novel opportunities in programmed self-assembly and nanofabrication.