The development of adhesives with superior optical and mechanical performance, solvent resistance, and reworkability is gaining increasing attention in recent years. However, traditional materials do not possess reprocessability and healing characteristics for sustainable development. Here, a superior dynamic polythiourethane (PTU) adhesive with high reprocessability was developed by introducing covalent adaptable networks (CANs). Specifically, dynamic thiocarbamate bonds (TCB) were used to prepare PTU CANs, which showed dramatically enhanced malleability and recyclability. The Young’s modulus of the material was 2.0 GPa and the tensile strength was 62.7 MPa. The reprocessing temperature of CANs was reduced to 80 °C while more than 90% of their mechanical properties were retained, even after being reprocessed several times. Moreover, the highly transparent and water-resistant PTU CANs featured an excellent bonding property and reworkability for various materials including glass, with a lap shear strength of 2.9 MPa, metal (5.1 MPa), and wood (6.3 MPa), compared with commercially available adhesives. Additionally, carbon fiber-reinforced composites constructed with PTU CANs were capable of being fully recycled and reused. Importantly, laminated glass with a toughened PTU–PU elastomer interface exhibited an outstanding impact fatigue-resistance behavior, sustaining thousands of impacts. These features demonstrate that PTU CANs show great potential as sustainable materials.

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