Macromolecular Chain Aggregation-Induced Multiscale Reinforcement for Strong and Antifatigue Hydrogels

Hydrogels have potential applications in artificial cartilage, tendons, and ligaments, while still facing great challenges in simultaneous improvement of strength, toughness, and fatigue resistance. In this work, strong, tough, and ionically conductive hydrogels are prepared via the macromolecular chain aggregation engineered multiscale reinforcement strategy. The tensile strength, fracture strain, fracture energy and fatigue threshold can reach values as high as 10.21 ± 0.79 MPa, 1942.84 ± 162.92%, 71.58 ± 4.23 kJ/m2, and 1040.12 J/m2, respectively. The hydrogels with ionic conductivity up to 1.45 S/m can be used as piezoresistive sensors for detection of various human body motions. This article provides a strategy for fabricating strong, tough, stretchable, and fatigue-resistant hydrogels with promising applications in flexible and wearable electronics.