Superelastic Biomass‐Based Carbon Aerogels Reinforced by Vein‐Like Networks and Pillar Structures for Piezoresistive Sensing, High‐Temperature Applications, and Supercapacitors

Abstract Biomass‐based carbon aerogels with tunable structures exhibit excellent compressibility and flexibility, serving as sustainable, cost‐effective materials for high‐performance piezoresistive sensors. However, achieving excellent integrated properties of superior fatigue resistance, ultra‐high compressibility, high sensitivity, low‐pressure detection limits, and wide linear sensing ranges remains a challenge. Herein, inspired by the leaf‐vein network structure and architectural pillar, a carbon aerogel with a “vein‐like network and pillar‐reinforced wavy layer structure” is developed. Benefiting from this structure, it enables exceptional fatigue resistance (96.7% stress retention and 99.1% height retention after 20000 compression cycles at 50% strain), which is second to none among the reported biomass‐based carbon aerogels. Meanwhile, its sensor integrates high linear sensitivity ( S = 59.70 kPa −1 at 0–100 Pa, S = 16.76 kPa −1 at 100–15000 Pa), a wide linear pressure range (0–15 kPa), an ultralow detection limit (0.186 Pa), and recoverable elasticity under extreme strain (99%), realizing the perfect performance of a piezoresistive sensor. Additionally, it exhibits excellent thermal insulation, flame resistance, and superior supercapacitive performance. These synergistic properties further enhance its applicability in motion monitoring, sensor units of aerospace, supercapacitors, and self‐powered wearable devices.