The new generation of carbon nanomaterials, represented by carbon nanotubes and graphene, have been the ideal reinforcement for metal matrix composites (MMCs) due to their excellent mechanical properties and unique structure. The strength of metal materials can be improved by means of material compounding. However, this method always compromises strength and toughness, which limits the development of high-performance composite materials and their industrial applications. Inspired by the “brick-and-mortar structure” of nacre in nature, bionic layered structure design is an effective means to solve this problem and fabricate lightweight, high-strength and super-toughness composite materials. In this paper, the fabrication technology of biomimetic layered carbon nanomaterials reinforced metal matrix composites was reviewed and some thoughts were put forward.