The remarkable progress in efforts to prepare conductive self-healing hydrogels mimicking human skin's functions has been witnessed in recent years. However, it remains a great challenge to develop an integrated conductive gel combining excellent self-healing and mechanical properties, which is derived from their inherent compromise between the dynamic cross-links for healing and steady cross-links for mechanical strength. In this work, we design a tough, self-healing, and self-adhesive ionic gel by constructing synergistic multiple coordination bonds among tannic acid-coated cellulose nanocrystals (TA@CNCs), poly(acrylic acid) chains, and metal ions in a covalent polymer network. The incorporated TA@CNC acts as a dynamic connected bridge in the hierarchically porous network mediated by multiple coordination bonds, endowing the ionic gels the superior mechanical performance. Reversible nature of dynamic coordination interactions leads to excellent recovery property as well as reliable mechanical and electrical self-healing property without any assistance of external stimuli. Intriguingly, the ionic gels display durable and repeatable adhesiveness ascribed to the presence of catechol groups from the incorporated tannic acid, which can be adhered directly on human skin without inflammatory response and residual. Additionally, the ionic gels with a great strain sensitivity can be employed as flexible strain sensors to monitor and distinguish both large motions (e.g., joints bending) and subtle motions (e.g., pulse and breath), which enable us to analyze the data on the user interface of smart phone via programmable wireless transmission. This work provides a new prospect for the design of the biocompatible cellulose-based hydrogels with stretchable, self-adhesive, self-healing, and strain-sensitive properties for potential applications in wearable electronic sensors and healthcare monitoring.

Conductive hydrogels are attracting tremendous interest in the field of flexible and wearable soft strain sensors because of their great potential in electronic skins, and personalized healthcare monitoring. However, conventional conductive hydrogels using pure water as the dispersion medium will inevitably freeze at subzero temperatures, resulting in the diminishment of their conductivity and mechanical properties; meanwhile, even at room temperature, such hydrogels suffer from the inevitable loss of water due to evaporation, which leads to a poor shelf-life. Herein, an antifreezing, self-healing, and conductive MXene nanocomposite organohydrogel (MNOH) is developed by immersing MXene nanocomposite hydrogel (MNH) in ethylene glycol (EG) solution to replace a portion of the water molecules. The MNH is prepared from the incorporation of the conductive MXene nanosheet networks into hydrogel polymer networks. The as-prepared MNOH exhibits an outstanding antifreezing property (−40 °C), long-lasting moisture retention (8 d), excellent self-healing capability, and superior mechanical properties. Furthermore, this MNOH can be assembled as a wearable strain sensor to detect human biologic activities with a relatively broad strain range (up to 350% strain) and a high gauge factor of 44.85 under extremely low temperatures. This work paves the way for potential applications in electronic skins, human−machine interactions, and personalized healthcare monitoring.

Healable, adhesive, wearable, and soft human-motion sensors for ultrasensitive human-machine interaction and healthcare monitoring are successfully assembled from conductive and human-friendly hybrid hydrogels with reliable self-healing capability and robust self-adhesiveness. The conductive, healable, and self-adhesive hybrid network hydrogels are prepared from the delicate conformal coating of conductive functionalized single-wall carbon nanotube (FSWCNT) networks by dynamic supramolecular cross-linking among FSWCNT, biocompatible polyvinyl alcohol, and polydopamine. They exhibit fast self-healing ability (within 2 s), high self-healing efficiency (99%), and robust adhesiveness, and can be assembled as healable, adhesive, and soft human-motion sensors with tunable conducting channels of pores for ions and framework for electrons for real time and accurate detection of both large-scale and tiny human activities (including bending and relaxing of fingers, walking, chewing, and pulse). Furthermore, the soft humanmotion sensors can be enabled to wirelessly monitor the human activities by coupling to a wireless transmitter. Additionally, the in vitro cytotoxicity results suggest that the hydrogels show no cytotoxicity and can facilitate cell attachment and proliferation. Thus, the healable, adhesive, wearable, and soft human-motion sensors have promising potential in various wearable, wireless, and soft electronics for human-machine interfaces, human activity monitoring, personal healthcare diagnosis, and therapy.

Flexible and degradable pressure sensors have received tremendous attention for potential use in transient electronic skins, flexible displays, and intelligent robotics due to their portability, real-time sensing performance, flexibility, and decreased electronic waste and environmental impact. However, it remains a critical challenge to simultaneously achieve a high sensitivity, broad sensing range (up to 30 kPa), fast response, long-term durability, and robust environmental degradability to achieve fullscale biomonitoring and decreased electronic waste. MXenes, which are two-dimensional layered structures with a large specific surface area and high conductivity, are widely employed in electrochemical energy devices. Here, we present a highly sensitive, flexible, and degradable pressure sensor fabricated by sandwiching porous MXene-impregnated tissue paper between a biodegradable polylactic acid (PLA) thin sheet and an interdigitated electrode-coated PLA thin sheet. The flexible pressure sensor exhibits high sensitivity with a low detection limit (10.2 Pa), broad range (up to 30 kPa), fast response (11 ms), low power consumption (10 −8 W), great reproducibility over 10 000 cycles, and excellent degradability. It can also be used to predict the potential health status of patients and act as an electronic skin (E-skin) for mapping tactile stimuli, suggesting potential in personal healthcare monitoring, clinical diagnosis, and nextgeneration artificial skins.

Robust, stretchable, and strain-sensitive hydrogels have recently attracted immense research interest because of their potential application in wearable strain sensors. The integration of the synergistic characteristics of decent mechanical properties, reliable self-healing capability, and high sensing sensitivity for fabricating conductive, elastic, self-healing, and strain-sensitive hydrogels is still a great challenge. Inspired by the mechanically excellent and self-healing biological soft tissues with hierarchical network structures, herein, functional network hydrogels are fabricated by the interconnection between a "soft" homogeneous polymer network and a "hard" dynamic ferric (Fe) cross-linked cellulose nanocrystals (CNCs-Fe) network. Under stress, the dynamic CNCs-Fe coordination bonds act as sacrificial bonds to efficiently dissipate energy, while the homogeneous polymer network leads to a smooth stress-transfer, which enables the hydrogels to achieve unusual mechanical properties, such as excellent mechanical strength, robust toughness, and stretchability, as well as good self-recovery property. The hydrogels demonstrate autonomously self-healing capability in only 5 min without the need of any stimuli or healing agents, ascribing to the reorganization of CNCs and Fe via ionic coordination. Furthermore, the resulted hydrogels display tunable electromechanical behavior with sensitive, stable, and repeatable variations in resistance upon mechanical deformations. Based on the tunable electromechanical behavior, the hydrogels can act as a wearable strain sensor to monitor finger joint motions, breathing, and even the slight blood pulse. This strategy of building synergistic "soft and hard" structures is successful to integrate the decent mechanical properties, reliable self-healing capability, and high sensing sensitivity together for assembling a high-performance, flexible, and wearable strain sensor.