Superior Biomimetic Nacreous Bulk Nanocomposites by a Multiscale Soft-Rigid Dual-Network Interfacial Design Strategy

Biomimetic bulk structural materials have been paid increasing attention for their huge application prospects. Integrating close-to-ideal, ultrathin, and flexible nanostructured units into high-performance nacreous bulk nanocomposites is worth considering yet remains challenging due to the elusive micro- and nano-interface connections. Here, by introducing amultiscale soft-rigid polymer dual-network interfacial design strategy that enables us to appropriately reinforce the nanoscale building blocks or their bridging, we can construct a type of nacreous bulk nanocomposites with tunable mechanical properties in the mild, eco-friendly, and highly efficient bottom-up assembly process. The resultant nanocomposites can achieve continuously reinforced mechanical transformation without experiencing environmentally threatening interfacial manipulation processes. This interfacial design strategy, supported by sufficient experiments and simulations, endows the assembled nacreous nanocomposite with superior mechanical enhancement and improved stability under high humidity and temperature conditions. Combined with the scalable assembly technique, it will pave the way for the design of high-performance biomimetic bulk nanocomposites for structural applications.