Recently, self-healing hydrogel bioelectronic devices have raised enormous interest for their tissue-like mechanical compliance, desirable biocompatibility, and tunable adhesiveness on bioartificial organs. However, the practical applications of these hydrogel-based sensors are generally limited by their poor fulfillment of stretchability and sensitivity, brittleness under subzero temperature, and single sensory function. Inspired by the fiber-reinforced microstructures and mechano-transduction systems of human muscles, a self-healing (90.8%), long-lasting thermal tolerant and dual-sensory hydrogel-based sensor is proposed, with high gauge factor (18.28) within broad strain range (268.9%), low limit of detection (5% strain), satisfactory thermosensation (−0.016 °C–1), and highly discernible temperature resolution (2.7 °C). Especially by introducing a glycerol/water binary solvent system, desirable subzero-temperature self-healing performance, high water-retaining, and durable adhesion feature can be achieved, resulting from the ice crystallization inhibition and highly dynamic bonding. On account of the advantageous mechanoreception and thermosensitive capacities, a flexible touch keyboard for signature identification and a “fever indicator” for human forehead’s temperature detection can be realized by this hydrogel bioelectronic device.

Electronic skin is driving the next generation of cutting-edge wearable electronic products due to its good wearability and high accuracy of information acquisition. However, it remains a challenge to fulfill the requirements on detecting full-range human activities with existing flexible strain sensors. Herein, highly stretchable, sensitive, and multifunctional flexible strain sensors based on MXene- (Ti3C2Tx-) composited poly(vinyl alcohol)/polyvinyl pyrrolidone double-network hydrogels were prepared. The uniformly distributed hydrophilic MXene nanosheets formed a three-dimensional conductive network throughout the hydrogel, endowing the flexible sensor with high sensitivity. The strong interaction between the double-network hydrogel matrix and MXene greatly improved the mechanical properties of the hydrogels. The resulting nanocomposited hydrogels featured great tensile performance (2400%), toughness, and resilience. Particularly, the as-prepared flexible pressure sensor revealed ultrahigh sensitivity (10.75 kPa-1) with a wide response range (0-61.5 kPa), fast response (33.5 ms), and low limit of detection (0.87 Pa). Moreover, the hydrogel-based flexible sensors, with high sensitivity and durability, could be employed to monitor full-range human motions and assembled into some aligned devices for subtle pressure detection, providing enormous potential in facial expression and phonation recognition, handwriting verification, healthy diagnosis, and wearable electronics.

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To meet critical requirements on flexible electronic devices, multifunctionalized flexible sensors with excellent electromechanical performance and temperature perception are required. Herein, lignin-reinforced thermoresponsive poly(ionic liquid) hydrogel is prepared through an ultrasound-assisted synthesized method. Benefitting from the electrostatic interaction between lignin and ionic liquid, the hydrogel displays high stretchability (over 1425%), excellent toughness (over 132 kPa), and impressive stress loading-unloading cyclic stability. The hydrogel strain sensor presents excellent electromechanical performance with a high gauge factor (1.37) and rapid response rate (198 ms), which lays the foundation for human body movement detection and smart input. Moreover, owing to the thermal-sensitive feature of poly(ionic liquid), the as-prepared hydrogel displays remarkable thermal response sensitivity (0.217°C-1) in body temperature range and low limit of detection, which can be applied as a body shell temperature indicator. Particularly, the hydrogel can detect dual stimuli of strain and temperature and identify each signal individually, showing the specific application in human-machine interaction and artificial intelligence. By integrating the hydrogel strain sensor into a wireless sensation system, remote motion capture and gesture identification is realized in real-time.

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Hydrogel is frequently used as a solid electrolyte for all solid‐state supercapacitors (SCs) because of its liquid‐like ion‐transport property and high conformability. However, due to the higher water content, the hydrogel electrolyte undergoes inevitable freezing and/or dehydration with climate change. Herein, polypyrrole/carbon all‐solid‐state SCs (PCSCs) were developed based on a hierarchical polypyrrole/carbon nanotube electrode and a highly stretchable double‐network polymer hydrogel electrolyte with LiCl/ethylene glycol as a mixed solvent. The PCSCs showed excellent electrochemical performance and cycle stability with a wide operating temperature. The specific capacitances could reach 202.2 and 112.3 mF cm−2 at current densities of 0.5 and 3.0 mA cm−2, respectively. Meanwhile, the PCSCs showed outstanding mechanical properties in maintaining a high areal capacitance under deformations of bending and tension. The excellent water retention of the device also ensured the stable electrochemical performance of PCSCs in a wide temperature range (30–80°C), which could potentially represent a reliable application in various harsh environments.