Evolution of Naturally Dried MXene‐Based Composite Aerogels with Flash Joule Annealing for Large‐Scale Production of Highly Sensitive Customized Sensors

MXene aerogels, known for good electrical properties, offer immense potential for the development of high‐sensitivity pressure sensors. However, the intrinsic challenges stemming from the poor self‐assembly capability and high hydrophilicity of MXene impede the natural drying process of MXene‐based hydrogels, thereby constraining their application on a large scale in sensor technology. Herein, a graphene‐assisted approach aimed at modulating the hydrophobicity and enhancing framework strength of MXene through a well‐designed prefreezing technique incorporating 3D spherical macroporous structures is proposed. This synergistic strategy enables the fabrication of naturally dried MXene aerogels across various size scales. Moreover, the integration of 3D spherical macroporous structures improves elasticity and electrical responsiveness of aerogels. Consequently, the aerogel sensor exhibits great performances, including high sensitivity (1250 kPa−1), low detection limit (0.4 Pa), wide frequency response range (0.1–8 Hz), and excellent stability (1000 cycles). This sensor proves adept at monitoring pressure signals ranging from lightweight paper to human motion. Additionally, the application of customized laser engraving endows aerogels with unique functionalities, such as compressibility and immunity to strain, stretchability and resistance to compression, as well as wind detection. Thus, the proposed approach holds significant promise as a scalable method for the mass production of aerogels with versatile applications. This work reports the naturally dried MXene‐based aerogels and their applications in highly sensitive piezoresistive sensors, where a systematic drying strategy is explored in detail, including the improvement of MXene sheet stiffness, control of hydrophobicity, and optimization of pore structure. Further combined with laser engraving, customized multifunctional sensors are developed.