▎ 摘　　要

Various approaches have been exploited to copy nacreous structure into human-made structural nanocomposites with similar structure and impressive mechanical performance. However, it is still facing a great challenge to produce large-sized, strong, and tough, biopolymer-based nanocomposite, especially for further scale-up in practical application. Herein, a large-sized and nacre-inspired nanocomposite paper can be successfully prepared via a simple evaporation-induced self-assembly technique, based on assembling hybrid graphene oxide/sodium alginate (GO/SA) building blocks. Through optimizing the lamellar hybrid interfacial interactions derived from hydrogen-bonding network, the nacre-inspired nanocomposite achieves a unique integration of high strength (up to 350.3 MPa) and high toughness (22.4 +/- 2.9 MJ m(-3)), are superior to natural nacre, almost all GO and SA-related composites, and many engineering materials. The hydrogen bond-property correlation, combined with a simple assembling technique, will provide a powerful path for the large-scale production of lightweight, biopolymer-based materials with excellent mechanical properties.