Programming Hydrogen Bonds for Reversible Elastic‐Plastic Phase Transition in a Conductive Stretchable Hydrogel Actuator with Rapid Ultra‐High‐Density Energy Conversion and Multiple Sensory Properties

Abstract Smart hydrogels have recently garnered significant attention in the fields of actuators, human‐machine interaction, and soft robotics. However, when constructing large‐scale actuated systems, they usually exhibit limited actuation forces (≈2 kPa) and actuation speeds. Drawing inspiration from hairspring energy conversion mechanism, an elasticity‐plasticity‐controllable composite hydrogel (PCTA) with robust contraction capabilities is developed. By precisely manipulating intermolecular and intramolecular hydrogen‐bonding interactions, the material's elasticity and plasticity can be programmed to facilitate efficient energy storage and release. The proposed mechanism enables rapid generation of high contraction forces (900 kPa) at ultra‐high working densities (0.96 MJ m⁻³). Molecular dynamics simulations reveal that modifications in the number and nature of hydrogen bonds lead to a distinct elastic‐plastic transition in hydrogels. Furthermore, the conductive PCTA hydrogel exhibits multimodal sensing capabilities including stretchable strain sensing with a wide sensing range (1–200%), fast response time (180 ms), and excellent linearity of the output signal. Moreover, it demonstrates exceptional temperature and humidity sensing capabilities with high detection accuracy. The strong actuation power and real‐time sensory feedback from the composite hydrogels are expected to inspire novel flexible driving materials and intelligent sensing systems.