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Flexible transparent supercapacitors (FTSs) have aroused considerable attention. Nonetheless, balancing energy storage capability and transparency remains challenging. Herein, a new type of FTSs with both excellent energy storage and superior transparency is developed based on PEDOT:PSS/MXene/Ag grid ternary hybrid electrodes. The hybrid electrodes can synergistically utilize the high optoelectronic properties of Ag grids, the excellent capacitive performance of MXenes, and the superior chemical stability of PEDOT:PSS, thus, simultaneously demonstrating excellent optoelectronic properties (T: ≈89%, Rs: ≈39 Ω sq−1), high areal specific capacitance, superior mechanical softness, and excellent anti‐oxidation capability. Due to the excellent comprehensive performances of the hybrid electrodes, the resulting FTSs exhibit both high optical transparency (≈71% and ≈60%) and large areal specific capacitance (≈3.7 and ≈12 mF cm−2) besides superior energy storage capacity (P: 200.93, E: 0.24 µWh cm−2). Notably, the FTSs show not only excellent energy storage but also exceptional sensing capability, viable for human activity recognition. This is the first time to achieve FTSs that combine high transparency, excellent energy storage and good sensing all‐in‐one, which make them stand out from conventional flexible supercapacitors and promising for next‐generation smart flexible energy storage devices.

Stretchable, self‐healable, and high‐capacity supercapacitors (SCs), as a state‐of‐the‐art energy storage technology, hold enormous potential in cutting‐edge wearable electronics. However, it is challenging to achieve excellent stretchability, superior self‐healing ability, and high specific capacitance in the whole device simultaneously. Herein, a new class of high‐capacity, stretchable, and self‐healing SCs with all‐in‐one structures is constructed by synergistically utilizing multiple cross‐linking effect and dynamic reversible non‐covalent bonding of a stretchable and self‐healing hydrogel electrolyte. The interlocking all‐in‐one structure leads to seamless contact as well as synchronous deformation and change between the electrodes and the electrolyte. Thus, by virtue of the stretchability and the self‐healing ability of the electrolyte, the whole devices exhibit both excellent stretchability (elongation at break of 1060%) and superior self‐healing ability (mechanically self‐healing efficiency of ≈80%). Moreover, by regulating the mass loading of the electrode materials along with the good interface contact of the all‐in‐one structure, the SCs also show high specific capacitance (109 mF cm−2). Their comprehensive performances are among the best in the ever‐reported all‐in‐one SCs. Thus, this work provides a feasible strategy for constructing high‐capacity, stretchable, and self‐healable SCs for smart wearable electronics.

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