The presence of arsenite [As(III)] in water poses a significant risk to both human health and the environment on a worldwide scale. This research focuses on a water-stable ferrocene (Fc)-encapsulated Ni metal−organic framework MOF (NiFc-MOF), which has the ability to remove As(III) from aqueous solutions while maintaining a neutral pH. Fc incorporation and the imidazole surface can enhance arsenite adsorption. Chelation and complexation are the two processes that contributed to the material's exceptional adsorption capacity, which was measured at 213.9 mg/g and was the highest recorded value for MOF materials. NiFc-MOF is capable of being reused for numerous cycles and removes As(III) in a selective manner, even when other competing ions are present. The adsorption behavior of NiFc-MOF was analyzed by using the Langmuir isotherm model, which was found to be the most applicable of the available options. Based on these findings, the NiFc-MOF seems to have a significant amount of promise as an effective adsorbent for the removal of As(III) from polluted water sources.