Chiral supramolecular assemblies hold great promise for advanced chiral materials and devices, but their low chiroptical activity limits practical applications. W e report hierarchical supramolecular assemblies with giant chiroptical activity and mechanical attributes, achieved through co-assembly of achiral amphiphilic unimolecular micelles and chiral additives. Chiral fibrillar assemblies emerge from the nanostructured environment imposed b y the micelles, driven by progressive chirality transfer via multiple hydrogen bonds between micelles and chiral additives. Integrating achiral luminescent molecules and nanocrystals into these assemblies leads t o full-color circularly polarized luminescence( CL)-active materials with high dissymmetry factors o f ~10-1. Surprisingly, a concentration-dependent chirality inversion is accessed via tailoring the co-assembly kinetics. Our strategy underscores the potential o f capitalizing o n unimolecular micelles to engineer high-performance hierarchical chiral structures and efficient CPL-active materials.