Natural nacre exhibits extraordinary strong and tough properties with its brick-and-mortar structure that was perfected after millions of years of evolution. Inspired by nacre's hierarchical structure, we fabricated multifunctional bioinspired nanocomposites of graphene oxide (GO) and montmorillonite (MMT) nanosheets with poly(vinyl alcohol) (PVA) via a vacuum-assisted filtration self-assembly process. By combining graphene oxide and montmorillonite with PVA, we demonstrated an effective synergistic toughening effect and obtained integrated strong and tough bioinspired nanocomposites. Furthermore, these nanocomposites show high fatigue-resistant properties, high electrical conductivity and good fire retardant properties. As such, they have promising potential in many applications, including flexible electrodes, flame retardant insulation and as aerospace materials. The technique developed here provides new insights for designing nanocomposites with a complex hierarchical structure that mimic nacre.