Multifunctional Superelastic, Superhydrophilic, and Ultralight Nanocellulose‐Based Composite Carbon Aerogels for Compressive Supercapacitor and Strain Sensor

Abstract Developing superelastic and superhydrophilic carbon aerogels with intriguing mechanical properties is urgently desired for achieving promising performances in highly compressive supercapacitors and strain sensors. Herein, based on synergistic hydrogen bonding, electrostatic interaction, and π–π interaction within regularly arranged layered porous structures, conductive carbon aerogels with cellulose nanofibrils (CNF), carbon nanotubes (CNT) and reduced graphene oxide (RGO) are developed via bidirectional freezing and subsequent annealing. Benefiting from the porous architecture and high surface roughness, CNF/CNT/RGO carbon aerogels exhibit ultralow density (2.64 mg cm –3 ) and superhydrophilicity (water contact angle ≈0° at 106 ms). The honeycomb‐like ordered porous structure can efficiently transfer stress in the entire microstructure, thereby endowing carbon aerogels with high compressibility and extraordinary fatigue resistance (10,000 cycles at 50% strain). These aerogels can be assembled into compressive solid‐state symmetric supercapacitors showing excellent area capacitance (109.4 mF cm –2 at 0.4 mA cm –2 ) and superior long cycle compression performance (88% after 5000 cycles at compressive strain of 50%). Furthermore, the aerogels reveal good linear sensitivity ( S = 5.61 kPa –1 ) and accurately capture human bio‐signals as strain sensors. It is expected that such CNF/CNT/RGO carbon aerogels will provide a novel multifunctional platform for wearable electronics, electronic skin, and human motion monitoring.