Anchoring Solvent Molecules onto Polymer Chains Through Dynamic Interactions for a Wide Temperature Range Adaptable and Ultra‐Fast Responsive Adhesive Organogels

Organogels are less explored toward on‐sink flexible and stretchable electronics compared to hydrogels, due to the challenges in simultaneously achieving biocompability, satisfactory mechanical properties, environmental‐adaptive adhesion capability, and fast stimuli‐response. Herein, it is shown that a boronate ester polymer organogel with dynamic covalent and hydrogen bonds formed between the polymer networks and organic solvents meets all the above requirements. This is achieved through the gelation of a polymer bearing with boronic acid, imidazolium salt, and amide groups (named QBAM) in ethylene glycol (EG). The strong interactions between the polymer chains and the EG not only improve the toughness of QBAMs, but also inhibit the volatilization of EG, leading to a wide temperature (−10 to 190 °C) adaptability. Due to the abundant hydrogen bonds and electrostatic interaction, QBAM organogels are highly adhesive to a variety of substrates. The presence of imidazolium salt endows QBAM organogels with promising ionic conductivity. Strain sensors fabricated with QBAM organogels fit well on human skin and exhibit the advantages of high strain sensitivity (GF = 9.049), fast response (≈60.4 ms), good cyclic stability, and broaden temperature adaptability. This work opens up a new avenue for the design of multifunctional and biocompatible organogels for on‐skin devices.