On‐skin electrodes function as an ideal platform for collecting high‐quality electrophysiological (EP) signals due to their unique characteristics, such as stretchability, conformal interfaces with skin, biocompatibility, and wearable comfort. The past decade has witnessed great advancements in performance optimization and function extension of on‐skin electrodes. With continuous development and great promise for practical applications, on‐skin electrodes are playing an increasingly important role in EP monitoring and human–machine interfaces (HMI). In this review, the latest progress in the development of on‐skin electrodes and their integrated system is summarized. Desirable features of on‐skin electrodes are briefly discussed from the perspective of performances. Then, recent advances in the development of electrode materials, followed by the analysis of strategies and methods to enhance adhesion and breathability of on‐skin electrodes are examined. In addition, representative integrated electrode systems and practical applications of on‐skin electrodes in healthcare monitoring and HMI are introduced in detail. It is concluded with the discussion of key challenges and opportunities for on‐skin electrodes and their integrated systems.

Traditional human emotion recognition is based on electroencephalogram (EEG) data collection technologies which rely on plenty of rigid electrodes and lack anti‐interference, wearing comfort, and portability. Moreover, a significant distribution difference in EEG data also results in low classification accuracy. Here, on‐skin biosensors with adhesive and hydrophobic bilayer hydrogel (AHBH) as interfaces for high accuracy emotion classification are proposed. The AHBH achieves remarkable adhesion (59.7 N m−1) by combining the adhesion mechanism of catechol groups and electrostatic attraction. Meanwhile, based on the synergistic effects of hydrophobic group rearrangements and surface energy reduction, the AHB‐hydrophobic layer exhibits 133.87° water contact angles through hydrophobic treatment of only 0.5 h. Hydrogen and electrostatic bonds are also introduced to form a seamless adhesive‐hydrophobic hydrogel interface and inhibit adhesion attenuation, respectively. With the AHBH as an ideal device/skin interface, the biosensor can reliably collect high‐quality electrophysiological signals even under vibration, sweating, and long‐lasting monitoring condition. Furthermore, the on‐skin electrodes, data processing, and wireless modules are integrated into a portable headband for EEG‐based emotion classification. A domain adaptive neural network based on the transfer learning technique is introduced to alleviate the effect of domain shift and achieve high classification accuracy.

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Electronic-skin (E-skin) has been investigated extensively for robotic tactile sensing. However, E-skin sensors based on flexible metamaterials are still challenging to achieve. Moreover, the implementation of E-skin sensor arrays in the actual monitoring of robotic grasping and manipulation conditions are rather limited due to the difficulty in data processing. Herein, highperformance E-skin strain sensors based on flexible auxetic metamaterials are reported, which endow the sensors with the capability of measuring both compressive (40%) and tensile (>80%) strain in a wide range and superior sensitivity, as compared with sensors without the structure. With perception data collected by the sensors, a generic method for real-time detection of unstable robotic grasping is established. Through this method, the complicated problem of processing large-scale arrayed sensor signals is simplified into the calculation of two indices, which extract both time and frequency domain characteristics of the signals. The total detection time (including sensor measurement response and data processing) can be as short as 100 ms, in line with human skin response in slippage perception. Accurate detections in real-time during various grasping and manipulation tasks are presented, demonstrating the great value of the sensors and the detection approach in robotic perception and dexterous manipulation.

Electronic skins (e‐skins) have gained tremendous attention in health monitoring and disease diagnosis. However, the accumulated sweat at the skin/e‐skin interface would compromise the comfort, reliability, and fidelity for long‐term monitoring. Here, inspired by the active liquid transport phenomenon in nature, a biomimetic gold/thermoplastic polyurethane/cellulose membrane (Au/TPU/CM) based e‐skin is reported that can “pump” perspiration from the interface immediately through the combination of gradient porosity and surface energy gradient. The resulting electrode possesses good conductivity (2.68 Ω sq–1), excellent flexibility (the resistance only fluctuated 1.1% and 0.4% after 10 000 bending cycles and 2500 tensile cycles, respectively), and outstanding water vapor transmission and water evaporation rate (2.2 and 7.1 times as much as that of cotton fabric, respectively). The ultrafast perspiration‐wicking capability not only improves the wearing comfort but also minimizes the measurement error of skin hydration and temperature due to perspiration, eliminates the risk of short circuit in sensor array, and reduces the noise level, significantly enhancing the accuracy and reliability of multimodal sensing in e‐skins. The design strategy may encourage more material and structure development in e‐skins with improved sweat tolerance.