IntroductionColloidal nanoparticles of metals, metal oxides, semiconductors, and metal-organic frameworks (MOFs) are of significant interest in both fundamental research and practical applications, due to their unique optical, electrical, and catalytic properties. [1][2][3] Small molecule-based wet-chemical colloidal synthesis of nanoparticles has undergone considerable progress in precise control over structural parameters of products, such as their size, shape, composition, crystal facet, and surface The synthesis of well-defined inorganic colloidal nanostructures using functional macromolecules is an enabling technology that offers the possibility of fine-tuning the physicochemical properties of nanomaterials and has contributed to a broad range of practical applications. The utilization of functional reactive polymers and their colloidal assemblies leads to a high level of control over structural parameters of inorganic nanoparticles that are not easily accessible by conventional methods based on small-molecule ligands. Recent advances in polymerization techniques for synthetic polymers and newly exploited functions of natural biomacromolecules have opened up new avenues to monodisperse and multifunctional nanostructures consisting of integrated components with distinct chemistries but complementary properties. Here, the evolution of colloidal synthesis of inorganic nanoparticles is revisited. Then, the new developments of colloidal synthesis enabled by functional macromolecules and practical applications associated with the resulting optical, catalytic, and structural properties of colloidal nanostructures are summarized. Finally, a perspective on new and promising pathways to novel colloidal nanostructures built upon the continuous development of polymer chemistry, colloidal science, and nanochemistry is provided. Functional Macromolecules