Hierarchical chiral supramolecular assemblies with strong and invertible chiroptical properties.

Supramolecular assemblies hold great promise for advanced chiral materials because of their structural diversity and dynamic features, but their low chiroptical activity limits practical applications. We report hierarchical supramolecular assemblies with giant chiroptical activity and mechanical attributes achieved through coassembly of achiral amphiphilic unimolecular micelles and chiral additives. Chiral fibrillar assemblies emerge from the nanostructured environment imposed by the micelles, driven by progressive chirality transfer through multiple hydrogen bonds between components. Integrating multifarious achiral luminescent molecules and nanocrystals into these assemblies leads to full-color circularly polarized luminescence-active materials with dissymmetry factors of ~10. A concentration-dependent chirality inversion is accessed through tailoring the coassembly kinetics. This strategy enables efficient red CPL, crucial for quantum and optical technologies.