Solvent Engineering of Thermo‐Responsive Hydrogels Facilitates Strong and Large Contractile Actuations

Abstract Thermo‐responsive hydrogels can generate the actuation force through volumetric transitions in response to temperature changes. However, their weak mechanical properties and fragile actuation performance limit robust applications. Existing approaches to enhance these properties have typically depended on additional components, leading to an unavoidable interference to the actuation performance. In this work, robust thermo‐responsive hydrogels are fabricated through solvent engineering. A particular solvent, N ‐methylformamide, interacts affinitively with the carbonyl group of N ‐isopropylacrylamide monomer, solubilizes the monomer with extremely high concentration, stabilizes chain propagation during polymerization, and greatly increases chain lengths and entanglements of the resulting polymer. The synthesized hydrogels are highly elastic, strong, and tough, displaying remarkable thermo‐responsive contractile actuation. The simple synthetic process can broaden its applicability in designing robust functional hydrogel applications.