Nacre consists of 95% of brittle calcium carbonate platelets and 5% of ductile biopolymer. Due to organic-inorganic components structured like a “brick-and-mortar”, the composite shows exceptional mechanical properties such as remarkably high fracture toughness and tensile strength. Because of these properties, nacre-mimetics hold great potentials for high mechanical performance and functional materials. In the presentation, we have fabricated nacre-like nanocomposites via vacuum filtration of montmorillonite (MMT) and cellulose nanofibers (CNFs) mixture. Although the composite exhibited higher strength and toughness than pure MMT and CNFs, we tried to improve the mechanical property by changing it into the ternary system. Polymer binders were further introduced to improve mechanical property of the composites. We compare nanostructures, chemical characteristics, and mechanical properties of the composites systematically.