Anisotropic nanoparticles are powerful building blocks for materials engineering. Unusual properties emerge with added anisotropy-often to an extraordinary degree-enabling countless new applications. For bottom-up assembly, anisotropy is crucial for programmability; isotropic particles lack directional interactions and can self-assemble only by basic packing rules. Anisotropic particles have long fascinated scientists, and their properties and assembly behavior have been the subjects of many theoretical studies over the years. However, only recently has experiment caught up with theory. We have begun to witness tremendous diversity in the synthesis of nanoparticles with controlled anisotropy. In this Perspective, we highlight the synthetic achievements that have galvanized the field, presenting a comprehensive discussion of the mechanisms and products of both seed-mediated and alternative growth methods. We also address recent breakthroughs and challenges in regiospecific functionalization, which is the next frontier in exploiting nanoparticle anisotropy.