Hierarchical Self‐Assembly of Adhesive and Conductive Gels with Anion‐Coordinated Triple Helicate Junctions

Abstract The fabrication of anion‐coordinated assemblies into functional soft materials remains a major challenge. To this end, four C 2 ‐symmetric anion‐binding ligands equipped with ortho ‐phenylene‐bridged bis(urea) and amine or amide ends were designed, which generated A 2 L 3 triple helical architectures upon self‐assembly with phosphate ions. Hierarchical intermolecular hydrogen bonds among the terminal amine/amide groups and urea moieties resulted in the formation of functional gels. The obtained gels were further applied for conductive adhesion between different surfaces, displaying excellent flexibility and selective wettability. The viscoelastic gels constructed from anion‐coordinated assemblies described in this work represent the first example of a new class of anion‐coordination‐driven smart materials.