Highly stretchable and highly resilient polymer-clay nanocomposite hydrogels were synthesized by in situ polymerization of acrylamide in the presence of pristine montmorillonite (MMT) or chitosan-treated MMT nanoplatelets at an elevated temperature. Both nanocomposite hydrogels can be stretched to a strain of no less than 1290%. The treatment of clay with chitosan improves the tensile strength, elongation at break, and energy at break of the nanocomposite hydrogel by 237%, 102%, and 389%, respectively, due to the strong chitosan-MMT electrostatic interaction and the grafting of polyacrylamide onto chitosan chains. Both hydrogels display excellent resilience with low hysteresis; with a maximum tensile strain of 50%, ultralow hysteresis is found, while, with a maximum strain of 500%, both hydrogels fully recover their original state in just 1 min. The superb resilience of the nanocomposite hydrogels is attributed to the strong interactions within the hydrogels brought by chain branching, multiple hydrogen bonding, covalent bonding, and/or electrostatic force. The hydrogels can be fabricated into different shapes and forms, including microfibers spun using pressurized gyration, which may find a variety of potential applications in particular in healthcare.
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