Inspired by the ultralight and structurally robust spider webs, flexible nanofibril‐assembled aerogels with intriguing attributes have been designed for achieving promising performances in various applications. Here, conductive polyimide nanofiber (PINF)/MXene composite aerogel with typical “layer‐strut” bracing hierarchical nanofibrous cellular structure has been developed via the freeze‐drying and thermal imidization process. Benefiting from the porous architecture and robust bonding between PINF and MXene, the PINF/MXene composite aerogel exhibits an ultralow density (9.98 mg cm−3), intriguing temperature tolerance from ‐50 to 250 °C, superior compressibility and recoverability (up to 90% strain), and excellent fatigue resistance over 1000 cycles. The composite aerogel can be used as a piezoresistive sensor, with an outstanding sensing capacity up to 90% strain (corresponding 85.21 kPa), ultralow detection limit of 0.5% strain (corresponding 0.01 kPa), robust fatigue resistance over 1000 cycles, excellent piezoresistive stability and reproductivity in extremely harsh environments. Furthermore, the composite aerogel also exhibits superior oil/water separation properties such as high adsorption capacity (55.85 to 135.29 g g−1) and stable recyclability due to its hydrophobicity and robust hierarchical porous structure. It is expected that the designed PINF/MXene composite aerogel can supply a new multifunctional platform for human bodily motion/physical signals detection and high‐efficient oil/water separation.

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Wearable pressure sensors are in great demand with the rapid development of intelligent electronic devices. However, it is still a huge challenge to obtain high-performance pressure sensors with high sensitivity, wide response range, and low detection limit simultaneously. Here, a polyimide (PI)/carbon nanotube (CNT) composite aerogel with the merits of superelastic, high porosity, robust, and high-temperature resistance was successfully prepared through the freeze drying plus thermal imidization process. Benefiting from the strong chemical interactions between PI and CNT and stable electrical property, the composite aerogel exhibits versatile and superior brilliant sensing performance, which includes wide sensing range (80% strain, 61 kPa), ultrahigh sensitivity (11.28 kPa–1), ultralow detection limit (0.1% strain, <10 Pa), fast response time (50 ms) and recovery time (70 ms), remarkable long-term stability (1000 cycles), and exceptional detection ability toward different deformations (compression, distortion, and bending). Furthermore, the composite aerogel also shows stable sensing performance after annealing under different high temperatures and good thermal insulation property, making it workable in various harsh environments. As a result, the composite aerogel is suitable for the full-range human motion detection (including airflow, pulse, vocal cord vibration, and human movement) and precise detection of the pressure distribution when it is assembled into E-skin, demonstrating its great potential to serve as a high-performance wearable pressure sensor.

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With the rapid development of artificial intelligence, high-performance flexible strain/pressure sensors with excellent wearing comfortability are in urgent demand. In this study, flexible conductive MXene/cellulose nanocrystal (CNC) coated thermoplastic polyurethane...

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