Tough hydrogels with rapid self-reinforcement

Most tough hydrogels are reinforced by introducing sacrificial structures that can dissipate input energy. However, because the sacrificial damage cannot rapidly recover, the toughness of these gels drops substantially during consecutive cyclic loadings. We propose a damageless reinforcement strategy for hydrogels using strain-induced crystallization. For slide-ring gels in which polyethylene glycol chains are highly oriented and mutually exposed under large deformation, crystallinity forms and melts with elongation and retraction, resulting both in almost 100% rapid recovery of extension energy and excellent toughness of 6.6 to 22 megajoules per cubic meter, which is one order of magnitude larger than the toughness of covalently cross-linked homogeneous gels of polyethylene glycol.