In Situ Crosslinked Supramolecular Self‐Healing Hydrogels for Multifunctional Motion Signal Transmission Devices

This work pioneers a transformative approach to flexible electronics by integrating supramolecular host‐guest interactions‐an innovative strategy to address the longstanding mechanical limitations of such devices. Most existing flexible electronic materials lack intrinsic self‐healing capability. When fractured during repeated deformation, they often suffer irreversible mechanical damage and a severe loss of electrical performance. Herein, A dual‐network hydrogel was rationally designed, where crosslinked cyclodextrin (Poly‐CD) was embedded into a polyacrylamide/2‐acrylamido‐2‐methylpropanesulfonic acid (PAM/AMPS) matrix, with networks interconnected via acrylate‐modified adamantane (Ad‐DA) and stabilized through photo‐initiated polymerization. This architecture delivers exceptional mechanical performance, enabling the hydrogel to stretch ∼15.5 fold of the original length and the tensile toughness of 0.3973 MJ/m 3 , while the Ad‐CD host‐guest inclusion imparts intrinsic self‐healing critical for durable wearable applications with the tensile stress self‐healing efficiency of 80.40%, as it allows damage recovery and sustained functionality. Further significance lies in the incorporation of MXene nanosheets, which drastically boost conductivity as 1.65 S/m, merging mechanical robustness with electrical functionality. Leveraging this multifunctional hydrogel, a flexible energy‐harvesting device for motion sensing was developed and it can generate an open‐circuit voltage of 540 V. Additionally, its excellent adhesiveness enabled use as a bio‐adhesive conductive gel for electromyography (EMG) tests. This research not only advances supramolecular hydrogel design but also demonstrates their pivotal role in next‐generation human‐computer motion information transmission, opening new avenues for flexible electronics.