Atomically defined, zero-dimensional magic-size clusters play pivotal roles in the nucleation and growth of semiconductor nanocrystals. Thus, they provide new opportunities to understand and to control nucleation and growth reactions beyond classical nucleation theory and to employ these reactions in the colloidal synthesis of increasingly complex and anisotropic nanomaterials with atomic level monodispersity. Both challenges require reliable determination of the exact structure and size of these ultrasmall and metastable nanoclusters. In this Perspective, we review and discuss the current challenges in analytics of magic-size clusters, in elucidating their formation mechanism, and in using them as next-generation reagents in colloidal chemistry.