Abstract: Natural nacre, one of the most studied biological structural materials with delicate hierarchical structures and extraordinary performance, has inspired the design and fabrication of artificial structural ceramics with high fracture toughness. However, to meet the diverse requirements of different applications, future structural materials must be multifunctional with superior mechanical properties, such as strength, hardness, and toughness. Herein, based on the matrix-directed mineralization method for producing biomimetic structural materials, we introduce nanoparticles with different inherent functions into the platelets of artificial nacre via the co-mineralization of aragonite and the nanoparticles. Besides their enhanced mechanical properties, the obtained artificial nacre materials also exhibit different functions depending on the type of the nanoparticles. To extend the versatility of this strategy, the effects of nanoparticles of different sizes and zeta potentials on mineralization are also analyzed. This universal strategy can be applied to the fabrication of other types of functionalized biomimetic structural ceramics that have potential applications in various fields, such as biomedical science.