High Strength, Healable, Recyclable Ionogel Capable of Long‐term Load Cycling

ABSTRACT Ionogels have attracted growing interest as stretchable conductive materials for applications in soft robotics, electronic skins, and wearable electronics. However, achieving a system that integrates mechanical strength, self‐healing, recyclability, and long‐term durability under cyclic loading remains a significant challenge. Traditional designs often lack effective energy dissipation pathways, leading to fatigue accumulation during cyclic deformation. In this study, polyurethane elastomers were synthesized with adipic dihydrazide (ADDH) and imidazolidinyl urea (IAU) as chain extenders, and subsequently complexed with ionic liquids to form PU–IL ionogels. The acylsemicarbazide groups in ADDH form robust hydrogen bonds, analogous to the hard β‐sheet nanocrystals in spider silk, while IAU introduces weaker hydrogen bonds that resemble the soft amorphous protein matrix. During stretching, the strong hydrogen bonds preserve structural integrity, while the weaker bonds reversibly break to dissipate energy. Consequently, the ionogels exhibit impressive mechanical properties, including a tensile strength of 12.6 MPa, toughness of 85.7 MJ m −3 , excellent long‐term cyclic load stability, and a broad strain sensitivity range (0.1%–200%). Additionally, the reversible hydrogen‐bonding network facilitates polymer segment reorganization, enabling efficient self‐healing and recyclability. This study proposes a hydrogen‐bonding‐enabled design strategy for high‐performance ionogels, paving the way for next‐generation flexible and wearable electronic applications.