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Nature provides many paradigms for the design and fabrication of artificialcomposite materials. Inspired by the relationship between the well-orderedarchitecture and biopolymers found in natural nacre, we present a facilestrategy to construct large-scale organic/inorganic nacre-mimetics withhierarchical structure via a water-evaporation self-assembly process. Throughhydrogen bonding, we connect Laponite-nanoclay platelets with each other usingnaturally abundant cellulose creating thin, flexible films with a localbrick-and-mortar architecture. While the aqueous solution displays liquidcrystalline textures, the dried films show a pronounced Young's modulus (9.09GPa) with a maximum strength of 298.02 MPa and toughness of 16.63 MJm-3. Interms of functionalities, we report excellent glass-like transparency alongwith exceptional shape-persistent flame shielding. We also demonstrate thatthrough metal ion-coordination we can further strengthen the interactionsbetween the polymers and the nanoclays. These ion-treated hybrid films exhibitfurther enhanced mechanical, and thermal properties as well as resistanceagainst swelling and dissolution in aqueous environments. We believe that oursimple pathway to fabricate such versatile polymer/clay nanocomposites can openavenues for inexpensive production of environmentally friendly, biomimeticmaterials in aerospace, wearable electrical devices, artificial muscle, andfood packaging industry.

A Facile Approach to Prepare Self-Assembled, Nacre-Inspired Clay/Polymer Nano-Composites