This study focuses on the feasibility of sustainably synthesized MIL-100(Fe) as an alternative to conventional desiccants, such as silica gel and zeolites, which have low adsorption capacity and poor thermal characteristics for air dehumidification. MIL-100(Fe), a metal–organic framework, shows promise due to its excellent adsorption and customizable thermal properties. However, its synthesis typically involves toxic materials and high temperature/pressure conditions, which restrict its bulk production for large-scale applications. This study aims to explore sustainable synthesis methods for MIL-100(Fe) using non-toxic materials and milder reaction conditions and investigate its material characteristics and dehumidification performance. Experimental analyses are carried out to measure adsorption isotherms, kinetics, sorption heat, activation energy, and cyclic stability, and numerical simulations are conducted in COMSOL Multiphysics platform to estimate dehumidification performance. The test results demonstrate that MIL-100(Fe) has a higher water adsorption capacity compared to silica gel, with a unique stepwise adsorption into its two types of mesoporous cages. Increased temperatures cause the adsorption and desorption isotherms to shift towards higher relative humidity levels. The heat of water adsorption and desorption ranges between 2630–2906 kJ/kg and 2763–2848 kJ/kg, respectively. MIL-100(Fe) demonstrates high stability and no significant loss in water uptake capacity. The simulated performance indicate that MIL–100(Fe) has superior reaction rates and is 82 % more effective than the silica gel rotary wheel dehumidifiers.