Ferroan brucite, Mg 1−X Fe X (OH) 2 (0.05 < x < 0.35) was a common mineral product preserved in serpentinized peridotites. Studying the evolution of Mg 1−X Fe X (OH) 2 with different doping amounts of Fe 2+ was beneficial to reveal the role of Fe 2+ in forming different kinds of evolution products and the reasonable utilization of Mg 1−X Fe X (OH) 2 resources. In this study, Mg 1−X Fe X (OH) 2 with x being 0.05, 0.1 0.15, 0.2, and 0.3 were successfully prepared, characterized, and structurally refined in detail. The evolution products of Mg 1−X Fe X (OH) 2 in the presence of H 2 O, CO 2 , and O 2 were clearly investigated to assess the evolution process and the role of Fe 2+ . The evolution products were mainly CO 3 2− intercalated MgFe-layered double hydroxides (MgFe−CO 3 2− -LDHs) and MgCO 3 •3H 2 O. The content of MgFe− CO 3 2−-LDHs in the evolution products increased with the Fe 2+ doping content increased. While the content of MgCO 3 •3H 2 O changed in the opposite direction and completely disappeared as the doping content of Fe 2+ was 20%. Accordingly, the evolution mechanism of Mg 1−X Fe X (OH) 2 was afforded based on various characterization and calculation on the deformation and system energy of the products by molecular simulation. In the evolution process, the oxidization of Fe 2+ to Fe 3+ in Mg 1−X Fe X (OH) 2 by O 2 forced the entrance of CO 3 2− into the interlayers. Meanwhile, high content of doping Fe 2+ in Mg 1−X Fe X (OH) 2 resulted in the easy formation of MgFe−CO 3 2− -LDHs. Correspondingly, the change of surface charge, magnetic property, and adsorption ability toward Congo red was tested after evolution.