Host molecules (α-CD) hierarchically thread onto the double grafts of the comb-copolymerEC-g-PCL-b-PEO from the outer block to the inner block in aqueous solution. Adjusting the molar ratio between α-CD and copolymer can induce these supramacromolecular complexes to dynamically and reversibly self-tune their fabrication from micelles (0-D) to cylinders (1-D) to vesicles (3-D) to sheets (2-D) like “living” assemblies.