Towards Dynamic but Supertough Healable Polymers through Biomimetic Hierarchical Hydrogen‐Bonding Interactions

Abstract A biomimetic (titin protein molecular structure) strategy is reported for preparing transparent and healable elastomers featuring supertoughness (345 MJ m −3 ) and high tensile strength (44 MPa) after self‐healing enabled by hierarchical (single, double, and quadruple) hydrogen‐bonding moieties in the polymer backbone. The rigid domain containing hierarchical H‐bonds formed with urethane, urea, and 2‐ureido‐4[1H]‐pyrimidinone groups leads to a durable network structure that has enhanced mechanical properties and is also dynamic for rapid self‐healing. Healable polymers with hierarchical hydrogen‐bonding interactions show excellent recoverability and high energy dissipation owing to the durable interaction between polymer chains. This biomimetic strategy of using hierarchical hydrogen bonds as building blocks is an alternative approach for obtaining dynamic, strong, yet smart self‐healing polymers for heavy‐duty protection materials and wearable electronics.