Materials with well-defined microstructure will embody a new generation of technologies; promoting photons to more efficiently perform the functions of today’s electronic circuitry. The desperate drive to craft precise microscopic architecture would come rapidly to a close if atoms could simply be blown up to micron sizes and assembled into the crystal structures that are found in naturally. Beyond this science fiction scenario, micron sized particles must be synthetically generated which mimic the activity of atomic species and efficiently serve as self-assembling building blocks. Generating colloidal suspensions that act as atoms means imbuing particles with both directionality and functionality, which is challenging due to their inherent isotropic nature. This work explores an overarching framework for colloidal synthesis, breaking down a variety of pathways to grow, combine, and react particle suspensions in both a reliable and scalable fashion. Using a direct analogy to synthetic chemistries’ inter- and intra-molecular reactions, novel interparticle reactions are described that are used to generate regular colloidal clusters with specified shapes, and then transformed into functional building blocks via intraparticle colloidal fusion reactions. Furthermore, the use of oppositely charged colloids as ion mimics is discussed, which are used to grow robust crystalline solids from common suspensions, encapsulating the aspirations of colloidal science today.