Versatile Graphene Oxide Hybrid Supramolecular Hydrogel Driven by Host–Guest Interaction Showing Excellent Mechanical and Sensing Properties and Photothermal Responsiveness

Functionalized hydrogels hold great promise in the field of advanced materials; however, the development of multifunctional integrated hydrogels remains a challenge. Herein, we report a hybrid supramolecular copolymerization strategy to prepare multifunctional and stimulus-responsive hydrogels from acrylamide (AM), a cucurbit[8]uirl (CB[8]) host–guest complex, and graphene oxide (GO) loaded with an initiator. The obtained hydrogels exhibit enhanced mechanical properties (ultrastretchability of 2922%, fracture strength of 103.1 kPa), similar to the modulus of human skin tissue (98.1 kPa). Moreover, these hydrogels exhibit remarkable self-healing efficiency (97%), self-adhesion, conductivity (1.69 mS/cm), and biocompatibility and manifest a triple stimulation response to strain, heat, and near-infrared light (NIR). The host–guest complex formed between CB[8] and the ionic guest 1-benzyl-3-vinylimidazolium bromide (G) acts as dynamic cross-linking, energy dissipation, self-healing, and conductivity agents in the hydrogel network. Simultaneously, the uniform dispersion of GO within the hydrogel by initiator loading bolsters mechanical and photothermal properties of the hydrogel. Notably, functioning as a wearable strain sensor, the hydrogel could effectively monitor various human body movements. Importantly, the host–guest interaction-mediated strain, temperature, and NIR-controlled hybrid hydrogel provide a versatile smart platform for potential applications in flexible electronics and biomedical fields.