Unlike the mechanisms behind their enhanced mechanical properties, application of artificial nacre-like materials has attracted very little attention from scholars. In this study, we designed a unique artificial nacre-like material that integrated outstanding mechanical properties and dielectric insulation properties by assembling MTM nanosheet and aramid nanofiber (ANF) through vacuum-assisted filtration. Compared with other nanocomposite films, the layered ANF/MTM nanocomposite film displayed superior mechanical properties (the tensile strength of similar to 126.5 MPa and elongation at break of similar to 2.56%) and dielectric insulation performance (77.2 kV/mm). In addition, it exhibited good transparency and flexibility. Therefore, this nanocomposite film has great potential for application in flexible electronics and high-voltage electrical insulation.