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Tooth enamel is composed of arrayed fluorapatite (FAP) or hydroxyapatite nanorods modified with Mg-rich amorphous layers. Although it is known that Mg2+ plays an important role in the formation of enamel, there is limited research on the regulatory role of Mg2+ in the synthesis of enamel-like materials. Therefore, we focus on the regulatory behavior of Mg2+ in the fabrication of biomimetic mineralized enamel-like structural materials. In the present study, we adopt a bioprocess-inspired room-temperature mineralization technique to synthesize a multilayered array of enamel-like columnar FAP/polymer nanocomposites controlled by Mg2+ (FPN-M). The results reveal that the presence of Mg2+ induced the compaction of the array and the formation of a unique Mg-rich amorphous-reinforced architecture. Therefore, the FPN-M array exhibits excellent mechanical properties. The hardness (2.42 ± 0.01 GPa) and Young’s modulus (81.5 ± 0.6 GPa) of the as-prepared FPN-M array are comparable to those of its biological counterparts; furthermore, the enamel-like FPN-M array is translucent. The hardness and Young’s modulus of the synthetic array of FAP/polymer nanocomposites without Mg2+ control (FPN) are 0.51 ± 0.04 and 43.5 ± 1.6 GPa, respectively. The present study demonstrates a reliable bioprocess-inspired room-temperature fabrication technique for the development of advanced high-performance composite materials.

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