Synergistic non‐covalent interactions enable high‐strength fluorescent supramolecular materials with water‐assisted self‐healing and remolding properties

Abstract Supramolecular materials, characterized by dynamic reversibility and responsiveness to environmental stimuli, have found widespread applications in numerous fields. Unlike traditional materials, supramolecular materials that rely on non‐covalent interactions can allow spontaneous reorganization and self‐healing at room temperature. However, these materials typically exhibit low strength due to the weak bonding energies of non‐covalent interactions. This study presents the development of a high‐strength self‐healing supramolecular material that combines multiple interactions including ionic bonding, hydrogen bonding, and coordination bonding. The material, formed by the aggregation of the negatively charged picolinate‐grafted copolymer (PCM) with positively charged hyperbranched molecules (HP), is further enhanced by Eu 3+ ion complexation. The resulting film exhibits a high modulus of 427 MPa, tensile strength of 10.5 MPa, and toughness of 14.7 MJ m −3 . Meanwhile, the non‐covalent interaction of this supramolecular material endows it with a self‐healing efficiency of 92% within 24 h at room temperature, as well as multiple remolding properties. The incorporation of lanthanide ions also imparts tunable fluorescence. This study not only provides insights into the development of high‐strength self‐healing materials but also offers new possibilities for the functionalization of supramolecular materials.