High‐Strength and Reprocessable Supramolecular Polydiketoenamine Network Materials for Sustainable Adhesives

Achieving both high strength and reprocessability in a single plastics material remains a fundamental challenge. Herein, we report the design and synthesis of novel supramolecular polydiketoenamine (PDK) network materials that were synergistically dual crosslinked by both the dynamic diketoenamine bonds and supramolecular cross-links (hydrogen-bonded benzene-1,3,5-tricarboxamide units). As a result, the PDK films exhibited a well-balanced combination of mechanical robustness and dynamic adaptability, achieving a high tensile strength of up to ∼77.21 MPa along with outstanding thermal reshaping and self-healing capabilities. Remarkably, beyond serving as strong structural films, the PDK plastic film exhibited superior performance as solid-state adhesives for diverse substrates-glass, metal, ceramic-exhibiting an enhanced lap-shear strength (up to ∼23.51 MPa) and retaining over 90% of its performance on glass after multiple reprocessing cycles. This work provides a promising strategy of integrating supramolecular cross-links into covalent adaptive network to construct high-performance, reprocessable network polymers that bridge the gap between the robustness of thermosets and the reprocessability of the thermoplastics.