Multi‐Modal Sensing Ionogels with Tunable Mechanical Properties and Environmental Stability for Aquatic and Atmospheric Environments

Abstract Ionogels have garnered significant interest due to their great potential in flexible iontronic devices. However, their limited mechanical tunability and environmental intolerance have posed significant challenges for their integration into next‐generation flexible electronics in different scenarios. Herein, the synergistic effect of cation‐oxygen coordination interaction and hydrogen bonding is leveraged to construct a 3D supramolecular network, resulting in ionogels with tunable modulus, stretchability, and strength, achieving an unprecedented elongation at break of 10 800%. Moreover, the supramolecular network endows the ionogels with extremely high fracture energy, crack insensitivity, and high elasticity. Meanwhile, the high environmental stability and hydrophobic network of the ionogels further shield them from the unfavorable effects of temperature variations and water molecules, enabling them to operate within a broad temperature range and exhibit robust underwater adhesion. Then, the ionogel is assembled into a wearable sensor, demonstrating its great potential in flexible sensing (temperature, pressure, and strain) and underwater signal transmission. This work can inspire the applications of ionogels in multifunctional sensing and wearable fields.