Stimuli‐Responsive Peptide Self‐Assembly to Construct Hydrogels with Actuation and Shape Memory Behaviors

Abstract Hydrogel actuators, capable of generating reversible deformation in response to external stimulus, are widely considered as new emerging intelligent materials for applications in soft robots, smart sensors, artificial muscles, and so on. Peptide self‐assembly is widely applied in the construction of intelligent hydrogel materials due to their excellent stimulus response. However, hydrogel actuators based on peptide self‐assembly are rarely reported and explored. In this study, a pH‐responsive peptide (MA‐FIID) is designed and introduced into a poly( N ‐isopropyl acrylamide) backbone (PNIPAM) to construct bilayer and heterogeneous hydrogel actuators based on the assembly and disassembly of peptide molecules under different pH conditions. These peptide‐containing hydrogel actuators can perform controllable bending, bucking, and complex deformation under pH stimulation. Meanwhile, the Hofmeister effect of PNIPAM hydrogels endows these peptide‐containing hydrogels with enhanced mechanical strength, ionic stimulus response (CaCl 2 ), and excellent shape‐memory property. This work broadens the application of supramolecular self‐assembly in the construction of intelligent hydrogels, and also provides new inspirations for peptide self‐assembly to construct smart materials.