High‐Adhesion Quadruple Hydrogen‐Bonded Ionogels: A Dual‐Function Platform for Gesture Recognition and Real‐Time <scp> NH ₃ </scp> Detection in Multiscenario

Ionogels have garnered significant attention in flexible sensing due to their outstanding mechanical properties, conductivity, and stability. However, establishing a robust and stable adhesive interface with various substrates remains a significant challenge. Herein, hydrogen‐bonded ionogels were synthesized through the self‐polymerization of hydrophobic ionic monomers. The introduction of hydrogen bonding effectively balances the intrinsic cohesive strength of the ionogels and their interfacial wettability, thereby enhancing adhesive strength. The optimal ionogels exhibited a tensile strength of 0.62 MPa, a modulus of 0.474 MPa, and an adhesive strength of 1208.3 kPa, surpassing most reported values for ionogels. Additionally, the ionogels retained superior electrical conductivity (44.78 mS cm −1 ) and excellent optical transparency (&gt;80%). A strain sensor fabricated from the ionogels demonstrated excellent sensitivity and stability, enabling the construction of a smart sensing glove capable of precise gesture recognition when integrated with deep learning algorithms. Intriguingly, the ionogels also exhibited selective recognition of ammonia (NH 3 ), with a detection limit (LOD) of 65 ppb. Leveraging these advantages, the integration of the ionogel with a wireless data acquisition and transmission module enables rapid, convenient, and real‐time NH 3 detection. This work presents an effective approach for developing highly adhesive ionogels, broadening their potential for practical applications.