The invention discloses an artificial nacre material with layered structure and preparation method thereof. The preparation method includes the following steps: uniformly mixing a carbonated cementitious material and water at a water-solid ratio of 0.3 to 1.2 to obtain a carbonated cementitious material suspension; treating the carbonated cementitious material suspension by a freeze-casting process to obtain a carbonated cementitious material coagulation with layered structure; treating the carbonated cementitious material coagulation with the layered structure by a freeze-drying process to obtain a carbonated cementitious material with layered structure; treating the carbonated cementitious material with layered structure by a carbonization process to obtain an artificial nacre material with layered structure. The obtained artificial nacre material with layered structure has higher fracture toughness and durability, and the preparation method has the advantages of low energy consumption, carbon dioxide fixation and environmental friendliness.