The metal-organic framework (MOF) MIL-68(In)-NH2 was tested for dye removal from wastewater and carbon capture gas separation. MIL-68(In)-NH2 was synthesized as a neat, supported MOF thin film membrane and as spherical particles using pyridine as a modulator to shape the morphology. The neat MIL-68(In)-NH2 membranes were employed for dye removal in cross-flow geometry, demonstrating strong molecular sieving. MIL-68(In)-NH2 particles were used for electrospinning of poylethersulfone mixed-matrix membranes, applied in dead-end filtration with unprecedented adsorption values. Additionally, the neat MOF membranes were used for H2/CO2 and CO2/CH4 separation.