Glucose‐Derived Circular Thermoset Platform Breaks the Industrial Trilemma of Recyclable Structural Polymers

ABSTRACT The long‐standing trilemma of scalable green synthesis, industrial processing compatibility, and balanced performance‐circularity represents the core barrier limiting real‐world deployment of recyclable thermosets. Here, we report an exogenous catalyst‐ and solvent‐free one‐pot strategy with ∼100% atom economy to fabricate glucose‐derived built‐in dynamic covalent thermosets from three industrial bulk feedstocks: glucose, maleic anhydride, and pentaerythritol tetrakis(3‐mercaptopropionate). The optimal formulation achieves an unprecedented balance between >130 d of room‐temperature shelf life (no gelation) and 2‐min gelation at 150°C, delivering engineering‐grade tensile strength up to 113 MPa, 17.5 MPa steel lap shear strength, and drop‐in compatibility with industrial vacuum‐assisted resin infusion for large carbon fiber composite manufacturing. We demonstrate complete room‐temperature closed‐loop recycling: nondestructive recovery of high‐value carbon fibers with full performance retention, and matrix degradation products (73.2%–83.1% isolated yield) upcyclable into high‐performance epoxy curing agents. Thermal reprocessing provides an additional reuse pathway for manufacturing scrap. Our cradle‐to‐grave life cycle assessment confirms 81.4% lower CO 2 ‐equivalent emissions than virgin bisphenol A epoxy carbon fiber composites. This work establishes a generalizable, industrially deployable paradigm for circular high‐performance thermosets, resolving the long‐standing trilemma impeding recyclable thermosets deployment.