Stretchable Multiresponsive Hydrogel with Actuatable, Shape Memory, and Self‐Healing Properties

Abstract Smart hydrogels with responsive behaviors have attracted tremendous attention. However, it is still a challenge to synthesize stretchable hydrogels capable of changing their original properties in response to multiple external stimuli. Here, integration of actuation function, shape memory, and self‐healing capability in a highly stretchable hydrogel under triple external triggers is achieved by rationally engineering multiple functional moieties. The hydrogel exhibits high stretchability (average relative strain (mm/mm) is >15) and excellent fatigue resistance during 100 loading cycles of 100% strain. Incorporating a moisture‐insensitive polymer film with the hydrogel, hydroactuated functionality is demonstrated. Moreover, shape memory and self‐healing abilities of the hydrogel are realized by the formation of ionic crosslinking or dynamic borate ester in conditions of multivalent cations and pH, respectively. Deformable plastic flowers are displayed in this work as a proof‐of‐concept, and it is believed that this smart hydrogel could be used in plenty of frontier fields, such as designing electronic devices, soft robotics, and actuators.