Hydrogen-bonded multi-mode liquid crystal elastomer actuators

As biomimicry advances, liquid crystal elastomers (LCEs) are gaining attention for their (multi-)stimuli-responsiveness and reversible shape morphing. Introduction of dynamic bonds into the LCEs provides versatile means towards programmable shape morphing and adaptation to environmental cues, and new designs for dynamic LCEs are actively sought for. Here, we present a supramolecular LCE that integrates shape memory programming, humidity sensitivity, and photochemical actuation. By utilizing hydrogen bonding crosslinks, the LCE gains shape memory functionality, enabling arbitrary shape programming and photochemical actuation. By breaking the supramolecular crosslinks <i>via</i> base treatment, the LCE becomes hygroscopic and humidity sensitive, yet maintains photochemical deformability. These two states enable different types of soft actuator demonstrations both in air and under water, adding to the versatility and programmability of light-driven shape-changing LCEs.