Conformation‐Mediated Energy Dissipation Enables High‐Damping and Environmentally Tolerant Ionogels for Flexible Sensing

ABSTRACT Addressing the intrinsic challenge of reconciling high damping performance with extreme environmental tolerance in soft materials, we propose a synergistic reinforcement strategy that integrates conformation‐change mediation with dynamic interfacial coupling for energy dissipation. Utilizing alkenylated cyclodextrin (CM) as a multifunctional structural unit, the system undergoes a stress‐induced conformational transition, establishing intrinsic energy‐dissipating units. Concurrently, host‐guest interactions bolster the interfacial stability of the ionic liquid, while thiol‐ene covalent crosslinking further optimizes interfacial compatibility. Moreover, the abundant multi‐hydroxyl sites cooperatively construct a multi‐tiered reversible hydrogen‐bonding network, culminating in an integrated crosslinked microstructure that enables homogeneous stress transfer and cascade energy dissipation. The resultant composite ionogel simultaneously achieves exceptional damping capacity (>94%), ultrahigh impact strength (>110 MPa), a low swelling ratio (<13.7%), outstanding low‐temperature tolerance (Tg < −78.8°C), and desirable mechanical properties, including a tensile strength of ∼7.5 MPa and a toughness of 26.9 MJ/m 3 . Through molecular dynamics simulations and comprehensive multi‐dimensional characterizations, we elucidate the conformation‐mediated microscopic energy‐dissipation mechanism. This work significantly broadens the application prospects of ionogels in impact protection, damping and energy absorption, extreme environments, and flexible wearable electronic sensing.