High Strength Polyurea Elastomers with Superior Room Temperature Self‐Healing, Recyclability, and Extreme‐Temperature Mechanical Robustness

Abstract Achieving simultaneous high strength, toughness, room temperature self‐healing, recyclability, and extreme‐temperature adaptability remains a critical challenge for thermoplastic elastomers (TPE). Here, a series of thermoplastic polyurea elastomers (IPDI‐D2000‐PPD) with hierarchical hydrogen‐bonding networks are synthesized using polyether amine (D2000) as soft segments, isophorone diisocyanate (IPDI) as hard segments, and p‐phenylenediamine (PPD) as chain extenders. By adjusting hard‐segment content, the materials exhibit outstanding room‐temperature properties, including tensile strength up to 38.6 MPa, toughness reaching 164.2 MJ m −3 , true stress of 354.0 MPa, and remarkable crack tolerance, whereby the notched sample can lift 48,600 times its own weight. The synergistic effects of flexible polyether chains and reversible hydrogen bonds endow the elastomers with 90% self‐healing efficiency at room temperature under trace ethanol and over 90% mechanical recovery after four recycling cycles. Importantly, they retain mechanical robustness across extreme temperatures, with strengths of 56.4 MPa at −50 °C and 14.3 MPa at 120 °C, and toughness of 143.6 and 98.6 MJ m −3 . Incorporation of ionic liquids further yields conductive ionogels for strain sensing. This work demonstrates a simple and versatile molecular design strategy, bridging performance gaps in multifunctional elastomers for sustainable, extreme‐temperature adaptability, and intelligent applications.