An Intrinsic Photothermal Supramolecular Hydrogel with Robust Mechanical Strength and NIR‐Responsive Shape Memory

Abstract Near Infrared (NIR)‐triggered shape memory hydrogels with promising mechanical strength hold immense potential in the field of biomedical applications and soft actuators. However, the optical and mechanical properties of currently reported hydrogels usually suffer from limited solubility and dispersion of commonly used photothermal additives in hydrogels, thus restricting their practical implementations. In this study, we report a set of NIR‐responsive shape memory hydrogels synthesized by polyaddition of diisocyanate‐terminated poly (ethylene glycol) (PEG), imidazolidinyl urea (IU) and p‐benzoquinone dioxime (BQDO). The introduction of IU, a hydrogen bond reinforcing factor, significantly enhances the mechanical properties of the hydrogels, allowing for their tunable ranges of the ultimate tensile strength (0.4‐2.5 MPa), elongation at break (210‐450%), and Young's modulus (190‐850 kPa). The unique hydrogels exhibit an intrinsic photothermal effect because of the covalently incorporated photothermal moiety (BQDO), and the photothermal supramolecular hydrogel shows controllable shape memory capabilities characterized by rapid recovery speed and high recovery ratio (> 90%). Our design would provide new possibilities for applying shape memory hydrogels in the field of soft actuators. This article is protected by copyright. All rights reserved