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Supramolecular plastics (SMPs) can be made mechanically robust, repairable, and recyclable, rendering themselves promising alternatives to their conventional predecessors to address environmental concerns. However, dense accumulations of noncovalent bonds generally lead to mechanical brittleness as well as intolerance toward heat and moisture. To resolve this issue, a simple strategy of preparing high‐performance SMP by constructing highly dense, but irregular hydrogen‐bond networks with hierarchical structures is proposed. The resultant SMP exhibits an outstanding combination of good comprehensive mechanical properties (high stiffness, strength, and toughness with ductile failure when fracturing), excellent dynamic behaviors (repairability and recyclability), and high tolerances toward moisture and high temperatures (as high as 90 °C). Additionally, the SMP also shows a high dielectric constant, exhibiting great potential for applications such as healable flexible touch screens and energy storage. Last, through structure characterizations and molecular dynamic simulation, this study provides a fundamental insight into the mechanism behind such high‐performances from nano‐ to micro‐scales, which is expected to inspire the design of a wide range of other SMPs that use different chemistries.
An ingenious construction of highly‐stacked, irregularly arranged, and hierarchical hydrogen‐bonding networks are designed to prepare a novel supramolecular plastic, which is colorless, transparent, robust, tough, humidity‐and heat‐resistant, and showed excellent repairability, recyclability, and high dielectric constant. The integration of these properties enables its potential applications in flexible touch screens and energy storage.