Passive indoor moisture control is a meaningful way to reduce HVAC operation and improve building energy efficiency. Metal-organic frameworks (MOFs) have been considered one of the most promising sorbent materials for passive indoor moisture control. However, the powder form of MOF is challenging to use in the built environment. Typical shaping methods like pellets, beads, and coating can lead to problems like partial pore blocking, insufficient mechanical stability, amorphization, and low material utilization. Here, we report a new sustainable MOF paper sheet comprising 25% cellulosic fibers and 75% MOF MIL-100(Fe) powder. The porous polymer matrix provides good support and fixation for MOF particles, so it’s more applicable in the built environment. The crystalline and pore structure characteristics of the MOF in the membrane are well preserved. Hydro characteristic test results show that MIL-100(Fe) paper sheet has high water vapor uptake, S-shape isotherm, mild regeneration condition, and high MBV. Then, a numerical model was developed to calculate the relation between a material’s MBV and its thickness. MIL-100(Fe) paper sheet with the most efficient thickness was applied as wallpaper in a building energy simulation model. The simulation result shows that the MIL-100(Fe) paper sheet is promising for passive indoor moisture control. It can remove about 45%-55% of the latent cooling load in most European climate types.