fabricated a montmorillonite clay (MTM)/poly(diallydimethylammonium) chloride polycation (PDDA) composite with nacre-like layer structure for the first time through sequential adsorption of organic and inorganic dispersions, [13] a typical layer-by-layer (LBL) method. The MTM/PDDA hybrid film with layer structure shows a fracture strength and strain of 105 MPa and 1%, respectively, approximately equal to that of nacre. Since then, more clay-based nacre-like films have been synthesized through the LBL method, and the mechanical properties are promoted by modifying the MTM [14] or crosslinking the polymer. [15] However, the thickness of the nacre-inspired films synthesized by the LBL method is limited to sub-10 µm as LBL is extremely time-consuming. [4] To increase the thickness of nacre-like films, efficient methods such as vacuum-assisted filtration, [16,17] electrophoretic-assisted deposition, [18] evaporation, [19,20] and dip-coating [21] have been developed in the following years. For example, the nacre-like MTM/poly(vinyl alcohol) (PVA) film with a thickness of over 200 µm, which is dozens of times thicker than films fabricated by LBL, can be synthesized through vacuum-assisted filtration, and its fracture strength and strain can be up to 160 MPa and 1%, respectively. [16] Recently, a much thicker clay-PVA composite (up to several millimeters) could be achieved by compressing and heating thin-layered films synthesized by evaporation. [22] Another typical method to produce bulk composites with layer structure is freeze-casting. [23][24][25][26] For instance, a lamellar Al 2 O 3 /poly(methyl methacrylate) (PMMA) composite with a size of dozens of centimeters showed a high combination of strength (flexural strength of 210 MPa) and toughness (32 MPa m 0.5 ), further surpassing the traditional structural materials. [23] In general, several methods have been developed since 2003 to synthesize nacre-inspired artificial composites with layer structures. However, the limitation of binary inorganic/organic hybrids still hinders further improvement of the mechanical properties of nacre-like artificial structural composites. [27] Recent progress in the synthesis of novel nacre-inspired structural materials, including ternary artificial nacre, artificial nacre reinforced by bridges, and those with a high content of hard phase, is discussed next, here, as a reference of the novel strategies for fabricating lighter, stronger, and tougher nacre-inspired structural materials. To give a comprehensive understanding, the perspective to develop next-generation lightweight and high-performance structural materials and their challenges is also included.For modern material engineering, one of the most ambitious goals is to develop lightweight structural materials with superior strength and toughness. Nacre, a typical biomaterial with high mechanical performance, has always inspired synthesis of high-performance structural composites. Here, the synthesis strategies for further enhancing the strength and toughness of novel nacre-insp...