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Fiber‐based multimodal sensors with electrical/optical signals are highly desired for next‐generation wearable electronics. Despite the remarkable progress in this area, achieving large‐scale knittable, washable, and self‐healing performance in fiber‐based multimodal sensors simultaneously remains a great challenge. Here, a smart fiber capable of exhibiting piezoresistive/luminescent properties based on an H‐bonding connected multilayered core–shell nanostructure is developed. The core principle of this design involves constructing strong interfacial interactions between the fiber layers, which results in a sensor with high sensitivity (gauge factor = 12383500), exceptional water resistance, and robust self‐healing properties (tensile strength 30.9 MPa, healing efficiency 72.9%). Unlike traditional fiber‐based sensors where elaborate nanostructures are prone to shedding during knitting, this strategy enables the fiber sensors with excellent knittability to be patterned in the fabric, improving both optical and electrical sensitivities. This work is anticipated to make a significant contribution to the further development of wearable electronic products and visual human–computer interaction electronic devices. [ABSTRACT FROM AUTHOR]

Smart fluorescent materials that can respond to environmental stimuli are of great importance in the fields of information encryption and anti‐counterfeiting. However, traditional fluorescent materials usually face problems such as lack of tunable fluorescence and insufficient surface‐adaptive adhesion, hindering their practical applications. Herein, inspired by the glowing sucker octopus, we present a novel strategy to fabricate a reversible fluorescent eutectogel with high transparency, adhesive and self‐healing performance for conformal information encryption and anti‐counterfeiting. Using anthracene as luminescent unit, the eutectogel exhibits photoswitchable fluorescence and can therefore be reversibly written/erased with patterns by non‐contact stimulation. Additionally, different from mechanically irreversible adhesion via glue, the eutectogel can adhere to various irregular substrates over a wide temperature range (−20 to 65 °C) and conformally deform more than 1000 times without peeling off. Furthermore, by exploiting surface‐adaptive adhesion, high transparency and good stretchability of the eutectogel, dual encryption can be achieved under UV and stretching conditions to further improve the security level. This study should provide a promising strategy for the future development of advanced intelligent anti‐counterfeiting materials. [ABSTRACT FROM AUTHOR]

• Scalable preparation of self-healing elastomers based on natural rubber. • Reversible ionic crosslinking results in excellent self-healing performance. • Nanostructured conductive network endows the sensor with high sensitivity. Flexible sensors which can recognize mechanical deformations have a great potential for next-generation smart devices. However, the defects of complicated fabrication steps, high cost and easily damaged gravely hinder their large-scale applications. Herein, we present a facile method to fabricate self-healing, highly sensitive strain sensors based on brominated natural rubber through ionically cross-linking and nanostructure design. The strong ionic bonding interaction of the components enables the elastomer with fast healing time (~10 s for mechanical healing and ~2 s for electrical healing) and satisfactory self-healing efficiency (93.98%). Furthermore, the designed nanostructured conductive network endows the sensor with high electrical sensitivity (GF ≈ 127) to realize the detection of both large- and small-strain human motions. This work provides great possibilities for the design and scalable manufacture of self-healing elastomers and wearable electronic devices. [ABSTRACT FROM AUTHOR]

Despite the tremendous advancement of intelligent robots, it remains a great challenge to integrate living organisms‐like multistimuli responsive actuation and excellent self‐healing ability into one single material system, which will greatly benefit and broaden the development of smart biomimetic materials. Herein, a novel self‐healable multistimuli responsive actuator is developed based on hierarchical structural design and interfacial supramolecular crosslinking. The resulting biomimetic actuator shows a record high photothermal efficiency (ηPT = 79.1%) and thermal conductivity (31.92 W m−1 K−1), and presents a superfast actuating response (near‐infrared light: 0.44 s; magnetic field: 0.36 s). In addition, the supramolecular crosslinking endows excellent self‐healing performance in both mechanical and actuating properties to the material. This biomimetic actuator with its hierarchical structure design provides great potential for various applications, such as artificial muscles, soft robotics, and biomedical microdevices. [ABSTRACT FROM AUTHOR]

[Display omitted] • Developed an effective strategy to achieve high-strength self-healing elastomer. • The TA-modified MXene is self-assembled in the matrix to form a network structure. • MXene networks impart composites with efficient photothermal conversion efficiency. • The prepared flexible actuator can realize actions such as crawling and grabbing. Self-healing ability is highly desired for flexible actuators that operate in dynamic and real-world environments, as these machines are vulnerable to mechanical damage. However, self-healing properties and mechanical strength are often difficult to combine at the same time. We report a synergistic enhancement strategy based on the ordered micro-nano structure and interfacial hydrogen bonding aggregation to achieve self-healing elastomer toughening. The hydrogen bonding interaction drives the MXene nanosheet to self-assemble into an interconnected network around the PU latex microsphere. Thanks to the synergy of dynamic physical networks and high-density interfacial hydrogen bonding, the composites with controllable room temperature self-healing efficiency (76.5–95.9%) and tensile strength (17.7–42.6 MPa). Furthermore, the MXene network structure of the composite endows the actuator with an efficient photothermal conversion efficiency, fast responsiveness, and even functional recovery. It is an effective strategy to achieve high-strength self-healing materials through hydrogen bonding connected MXene network and interfacial hydrogen bonding aggregation, which is expected to be applied to other flexible devices, such as flexible sensors and electromagnetic shielding. [ABSTRACT FROM AUTHOR]