Supramolecular Ionogels Tougher than Metals

Abstract Common natural and synthetic high‐strength materials (such as rubber, plastics, ceramics, and metals) undergo the occurrence of poor deformability. Achieving high strength and large deformation simultaneously is a huge challenge. Herein, high‐strength ionogels are developed through the synergy of force‐induced crystallization and halometallate ionic liquid created supramolecular ionic networks. The prepared poly(vinyl alcohol)/halometallate ionic liquid ionogels show excellent mechanical properties, including ultimate fracture stress (63.1 ± 2.1 MPa), strain (5248 ± 113%), and unprecedented toughness (1947 ± 52 MJ m −3 ), which is much higher than that of most metals and alloys. Furthermore, the ionogels can achieve reversibility by water to realize green recovery and restoration of damaged mechanical properties.