Epoxy nanocomposites combining high toughness with advantageous functional properties are needed in many fields. However, fabricating high-performance homogeneous epoxy nanocomposites with traditional methods remains a great challenge. Nacre with outstanding fracture toughness presents an ideal blueprint for the development of future epoxy nanocomposites. Now, high-performance epoxy-graphene layered nanocomposites were demonstrated with ultrahigh toughness and temperature-sensing properties. These nanocomposites are composed of ca. 99 wt % organic epoxy, which is in contrast to the composition of natural nacre (ca. 96 wt % inorganic aragonite). These nanocomposites are named an inverse artificial nacre. The fracture toughness reaches about 4.2 times higher than that of pure epoxy. The electrical resistance is temperature-sensitive and stable under various humidity conditions. This strategy opens an avenue for fabricating high-performance epoxy nanocomposites with functional properties.