A Strategy Inspired by the Cicada Shedding Its Skin for Synthesizing the Natural Material NaFe(3)S(5)·2H(2)O

Sulfide minerals hold significant importance in both fundamental science and industrial advancement. However, certain natural sulfide minerals, such as NaFe(3)S(5)·2H(2)O (NFS), pose great challenges for exploitation and synthesis due to their high susceptibility to oxidation. To date, no successful precedent exists for synthesizing NFS. Here, a novel approach to synthesizing low‐cost and pollution‐free NFS with high stability using the high‐pressure hydrothermal method based solely on knowledge of its chemical formula is presented. Moreover, an innovative strategy inspired by the cicada's molting process to develop unstable natural materials is proposed. The mechanical, thermal, optical, electrochemical, and magnetic properties of the NFS are thoroughly investigated. The storage of lithium, sodium, and potassium ions is primarily concentrated in the gap between (0 0 1) crystal planes. Additionally, as a catalyst for hydrogen evolution reaction (HER) at 10 mA cm(−2), micron‐sized NFS exhibits an excellent overpotential of 6.5 mV at 90 °C, surpassing those of reported HER catalysts of similar size. This research bridges the gap in the sulfide mineral family, overcomes limitations of the high‐pressure hydrothermal method, and paves the way for future synthesis of natural minerals, lunar minerals, and Martian minerals.