Strong, Hydrophobic, and Recyclable Materials Enabled by Nacre‐Like Multiple Interactions

ABSTRACT Achieving recyclable materials that simultaneously exhibit high mechanical strength and long‐lasting hydrophobicity remains a fundamental challenge, as dynamic or supramolecular systems typically suffer from compromised robustness or water resistance. Here, we report a layered material that integrates nacre‐like multiple interactions to overcome this trade‐off. The material is constructed from vermiculite nanosheets and a functional copolymer through evaporation‐induced assembly followed by thermal annealing, which triggers a ring‐closing transformation of polymer side chains. This process generates π–π interactions and hydrogen‐bonding networks that impart durable hydrophobicity, while strong Al─O─C coordination bonds at the organic–inorganic interface enable efficient load transfer and high mechanical strength (≈ 154 MPa). Importantly, these interactions are selectively and reversibly disrupted via an ammonia‐mediated ring‐opening reaction, allowing the material to be chemically cleaved and reprocessed into films with near‐original performance. The resulting system exhibits a rare combination of high strength, stable hydrophobicity (water contact angle ≈ 95°), and closed‐loop recyclability. This work establishes a biomimetic strategy for synergistically integrating multiple interactions in confined architectures, offering a general design principle for next‐generation sustainable structural materials.