Lotus-Root-Fibril-Inspired Strong, Tough, and Recyclable Poly(vinyl alcohol) Plastic Enabled by a Self-Assembled...

High-performance plastics combining high strength, superior toughness, and robust recyclability are highly desired but limited by intrinsic polymer constraints. Here, we report a high-performance poly(vinyl alcohol) (PVA) plastic enabled by a bio-inspired energy dissipation mechanism via an in situ self-assembly strategy. Integrating one-dimensional supramolecular microtubules with ordered multi-level pore channels into the PVA matrix creates a biomimetic "lotus-root-fibril" architecture that confines and pre-aligns polymer chains. Under load, energy hierarchically, initial dissociation of weak interlayer bonds within microtubules leads to controlled fragmentation, followed by extensive sliding and parallel alignment of confined PVA chains. This fibrous-bridge toughening yields a tensile strength of 94 MPa, strain of 760%, and an unprecedented toughness of 570.6 MJ m-3. The dynamic supramolecular microtubules grant the material excellent thermal/humidity resistance and closed-loop recyclability through reversible dissociation-reassociation. This simple, cost-effective method provides a scalable paradigm for designing sustainable ultratough plastics by incorporating supramolecular frameworks into existing commercial polymers.