Woven Crosslinks and Multiple Noncovalent Interactions Enabled an Ultratough, Highly Stretchable, and Recyclable Ionogel

Ultratough, highly stretchable, and self-healable ionogels are urgently desired due to their unique properties such as intrinsic ionic conductivity, low volatility, and high thermal stability. However, low strength and toughness still hinder the practicality of existing ionogels. Inspired by the spider silk microstructure, we proposed a strategy that simultaneously introduced woven crosslinks and multiple noncovalent interactions in a polymeric network to produce ionogels with excellent mechanical properties. Both woven crosslinks and noncovalent interactions dissipated energy to endow ultrahigh toughness to the ionogel. Additionally, the rigid nature of woven crosslinks enhanced the ionogel strength. Therefore, the ionogel exhibited high toughness (82.02 MJ m -3 ) and fracture energy (808.7 kJ m -2 ), healability, and recyclability. The toughness and fracture energies were superior to most previously reported ionogels. Moreover, this ionogel responded well to strains, indicating its potential use as a strain sensor. This strategy could lead to the production of other ionogels and hydrogels with intriguing mechanical properties.