Gelator-Enhanced Organohydrogels with Switchable Mechanics and High-Strain Shape-Memory Capacity

Hydrogels and organogels, as two crucial representatives of soft materials, have attracted immense interest. However, they develop independently along two parallel lines, and these gels with single networks have their inherent drawbacks. For example, hydrogels tend to freeze, and organogels are usually brittle. Herein, organogels were incorporated into a hydrogel matrix for the synthesis of organohydrogels GOHs through polymerization in Pickering emulsion. The rigid organogel domains contribute to enhancing the strength of organohydrogels. Besides this, the organogels derived from 12-HAS self-assembly behavior exhibit a gel–sol transition when the temperature reaches 70 °C, thus leading to a thermo-softening behavior in the GOHs. Due to the phase transition of organogel domains and the elastic hydrogel network, the resultant organohydrogels demonstrate high-strain shape-memory performance (over 1000%) which could help achieve full recovery in seconds. Consequently, GOHs are endowed with the potential of practical application in soft robots, wearable devices, and biological materials.