CO₂‑Switchable Supramolecular Block Glycopolypeptide Assemblies

A novel supramolecular block glycopolypeptide, designed to have the viral building blocks and be sensitive to CO₂, a physiological stimulus, was prepared via the orthogonal coupling of two end-functionalized biopolymers, dextran with β-cyclodextrin terminal (Dex-CD) and poly­(l-valine) with a benzimidazole tail (BzI-PVal), respectively, driven by the end-to-end host–guest interactions. Due to the CO₂-cleavable CD/BzI connection, both the vesicular and fibrous aggregates of this supramolecular block copolymer self-assembled in aqueous solution can undergo a reversible process of disassembly upon “breathing in” CO₂ and assembly upon “breathing out” CO₂, which mimics, to some extent, the disintegration and construction of viral capsid nanostructures.