Capturing formaldehyde (HCHO) from indoor air with porous adsorbents still faces challenges due to their low uptake capacity, difficult regeneration, and especially, the sorption capacity reduction that is caused by the competitive adsorption of H₂O when exposed to a humid atmosphere. In this work, MIL-101 is modified with ethylenediamine (ED) on its open-metal sites to substantially improve the HCHO adsorption properties. The HCHO uptake capacity of modified MIL-101 can be up to 5.49 mmol g⁻¹ in this study, which is among the highest-levels of various adsorbents reported thus far. Moreover, this modification both improved the material's recyclability and water resistibility, allowing for cyclic and selective tests with stable adsorption capacities, revealing the potential utility of amine-modified MOFs for indoor air purification.