The strength and toughness of materials are predominantly attributed to the structure-related stress distribution and energy dissipation in the deformation and damage process. Inspired by the hierarchical structure of nacre, the ternary structure artificial nacre composite films composed of homophonous dimensional hierarchy graphene oxide (GO) sheets and polyvinyl alcohol (PVA) were designed and prepared via the dry-spinning process. It demonstrates that there is a mechanical synergistic effect of the dimensional hierarchy GO sheets that can improve the stress distribution (suppress and disperse the local stress concentration regions) and increase the energy dissipation (trigger more crack deflection), thus improving the toughness on the premise of ensuring excellent strength of the films. Based on the dry-spinning and lamination assembly process, large-size bulk composites with excellent mechanical properties constructed by these films can be obtained and are expected to achieve mass production, which has great potential applications in aerospace, automobile, biomedical, and energyindustries.