Tough and Recyclable Phase-Separated Supramolecular Gels via a Dehydration–Hydration Cycle

[Image: see text] Hydrogels are compelling materials for emerging applications including soft robotics and autonomous sensing. Mechanical stability over an extensive range of environmental conditions and considerations of sustainability, both environmentally benign processing and end-of-life use, are enduring challenges. To make progress on these challenges, we designed a dehydration–hydration approach to transform soft and weak hydrogels into tough and recyclable supramolecular phase-separated gels (PSGs) using water as the only solvent. The dehydration–hydration approach led to phase separation and the formation of domains consisting of strong polymer–polymer interactions that are critical for forming PSGs. The phase-separated segments acted as robust, physical cross-links to strengthen PSGs, which exhibited enhanced toughness and stretchability in its fully swollen state. PSGs are not prone to overswelling or severe shrinkage in wet conditions and show environmental tolerance in harsh conditions, e.g., solutions with pH between 1 and 14. Finally, we demonstrate the use of PSGs as strain sensors in air and aqueous environments.