From Carbon Units to Architectures: Self-Assembly of Carbon Nanomaterials

Carbon’s diverse bonding configurations give rise to an exceptional range of nanostructures. These discoveries have inspired intensive research into carbon nanomaterials and their self-organization into functional architectures. This review traces the evolution of carbon nanomaterials and focuses on three representative structural units: fullerenes, carbon dots, and carbon nanotubes. Each class demonstrates unique physicochemical properties and self-assembly behaviors driven by noncovalent interactions such as π–π stacking, hydrogen bonding, and van der Waals forces. Representative studies are examined to illustrate how molecular design, surface functionalization, and solvent conditions guide these nanoscale units into ordered films, gels, and networks.  Finally, the challenges and perspectives for achieving precise control over the hierarchical assembly of carbon nanomaterials are discussed, aiming to advance their applications in optoelectronics, sensing, and biomedicine.