Remalleable, Healable, and Highly Sustainable Supramolecular Polymeric Materials Combining Superhigh Strength and Ultrahigh Toughness

the compression molding method. Compared to the conventional solution casting method for the fabrication of PVA-based thin films, the as-developed strategy allows large-scale production of bulk TA-PVA composites. The TA-PVA composites consist of interpenetrating three-dimensional supramolecular TA-PVA clusters. Such a structural feature, revealed by computational simulations, is crucial for the integrated superhigh strength and ultrahigh toughness of the material. The biodegradable TA-PVA composites are remalleable for multiple generations of recycling and healable after break, at room temperature, by the assistance of water to activate the reversibility of the hydrogen bonds. The TA-PVA composites show high promise as sustainable substitutes for conventional plastics because of their remalleability, healability, and biodegradability. The integrated superhigh strength and ultrahigh toughness of the TA-PVA composites ensure their high reliability and broad applicability.