▎ 摘　　要

Inspired by the hierarchical structure of nacre and the robust adhesive ability of mussel threads, graphene oxide-polydopamine (GO-PDA) nanocomposites are designed and synthesized to achieve enhanced mechanical properties and to provide additional functionalities. Here we report a joint experimental/computational investigation of GO-PDA nanocomposites, proposing a probable chemical reduction mechanism of PDA to convert GO to reduced GO (rGO), which helps increase the electrical conductivity. The most stable chemical connection between PDA and GO is also proposed. Our artificial nacre-like GO-PDA nanocomposites are shown to have higher tensile strength and toughness compared to natural nacre. The pulling tests conducted by molecular dynamics simulations, which are supported by our experiments, reveal that the enhanced mechanical strength of GO-PDA nanocomposites mainly originates from the additional non-covalent interactions provided by PDA. The humidity-driven shrinking mechanism of GO-PDA nanocomposites due to non-uniform stresses on the GO-PDA sheets is also discovered in our simulations and supported by our experiments. The findings in this work can help improve and tune the properties of GO-PDA nanocomposites and might also apply to other 2D materials.