Sensing bioelectrical signals paves a way for knowing the health and mental status, providing important clinical information about subjects' physiological and psychological activities. [1] Common bioelectrical signals include electromyogram (EMG), electrocardiogram (ECG), electrooculogram (EOG), and electroencephalogram (EEG). EMG is conducive to explore the activities of nerves and muscles. ECG signals, originating from heart, show the information related to cardiac function. EOG can help to recognize eye diseases. EEG is capable of showing complex neural activities in the brain. [2][3][4][5] Furthermore, bioelectrical signals could integrate with human-machine interfaces (HMI), such as prosthetic control, emotion recognition, eye movement tracking, virtual reality (VR), and augmented reality (AR). [6][7][8][9] So far, various bioelectrodes have been developed for recording bioelectrical signals, but it is still challenging to acquire high-quality, stable, and long-term signals. [10,11] Human skin/tissue will deform during body motion, which means that human skin/tissue has to withstand strain. Conventional bioelectrodes are mainly gel electrodes (Ag/AgCl electrodes) and dry electrodes made of metals (e.g., Au, Ag, Cu). Due to the mechanical mismatch with human skin/tissue, they are unable to continuously recording signals. In addition to, long-term use of such electrodes would cause skin irritation. Stretchability is a critical property to ensure bioelectrodes to work normally despite the deformation of human skin/tissue. Lots of interest is devoted to the fabrication of stretchable electrodes. [12][13][14][15][16] These electrodes need to possess matched modulus to adapt to the uneven surface of human skin/tissue. In addition to the mechanical properties, excellent conductivity, adhesion to skin, and biocompatibility are necessary. Furthermore, breathability and self-healing are also the properties people pursuing for. [17] Emerging materials used for bioelectrodes include conductive polymers, conductive hydrogels, carbon materials (e.g., graphene, carbon nanotubes), liquid metals, elastomer composites, etc. [18][19][20][21] Conductive polymers are kinds of organic conjugated polymers with heterocycle, whose conductivity stems from conjugated main chains of delocalized electron/hole. By combining the advantages of both metals and polymers, conductive polymers are easy for fabrication and structure modification. Among them, poly(3,4-ethylenedioxythiophene) (PEDOT) has attracted heightened interest due to its excellent conductivity, optical transmittance in the visible region, thermostability, relatively low redox potential, etc. Nevertheless, its insolubility in water hinders further development. It can be overcome by introducing polyelectrolyte like poly(styrenesulfonate) (PSS) into PEDOT matrix. PSS acts as both dopant and stabilizer by a charge balance mechanism. Since the problem of insolubility in water has been solved, PEDOT becomes the most successful commercial polyelectrolyte. [22] Figure 1 shows the s...