Rapid improvement of wearable electronics stimulates the demands for the matched functional devices and energy storage devices. Meanwhile, wearable microsystem requires every parts possessing high compressibility to accommodate large-scale mechanical deformations and complex conditions. In this work, a general carbon nanotube-polydimethylsiloxane (CNT-PDMS) sponge electrode is fabricated as the elementary component of the compressible system. CNT-PDMS sponge performs high sensitivity as a piezoresistance sensor, which is capable of detecting stress repeatedly and owns great electrochemical performance as a compressible supercapacitor which maintains stably under compressive strains, respectively. Assembled with the piezoresistance sensor and the compressible supercapacitor, such highly compressible integrated system can power and modulate the low-power electronic devices reliably. More importantly, attached to the epidermal skin or clothes, it can detect human motions, ranging from speech recognition to breathing record, thus showing feasibility in real-time health monitor and human-machine interfaces.

Bending and pressure sensors are very essential for evaluating external stimuli in human motions; however, most of them are separate devices. Here, two orthogonal carbon nanotube–polyurethane sponge strips (CPSSs) are used, each of which has different resistances when bent or pressed, to fabricate a multi‐functional stretchable sensor capable of detecting omnidirectional bending and pressure independently. Due to the shape of the strip, the resistance of CPSS changes differently when bent along different directions. Based on this feature, two perpendicular CPSSs can reflect information of both bending distance and bending direction. After basic measurement data are obtained, a function set can be formulated to calculate bending distance and bending direction simultaneously. The errors of bending distance and bending angle can be controlled to less than 4%. With the help of the triboelectric effect, which only happens when the device is pressed, the sensor can differentiate bending and pressure effectively, ensuring the device works in complex situations.

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