Metal organic framework materials (MOFs) are a classic three-dimensional porous crystalline materials formed by the assembly of metal ions or metal clusters and organic ligands. They have large specific surface areas, uniform pore size distributions, unsaturated metal active sites, and many other advantages. The introduction of other functional materials through functional group modification or doping can give MOFs more excellent performance, which is of great significance for improving the ability of a single MOFs material to remove pollutants in water. In this paper, MIL-53(Fe) and Br-MIL-53 (Fe) were synthesized to adsorb methyl orange from organic dyes. The results show that Br-modified MIL-53(Fe) exhibits higher adsorption performance than the original MIL-53(Fe). The effect of time, pH value, temperature, and dosage on adsorption performance of Br-MIL-53(Fe) have been studied. Moreover, it is also found that the MOF material is a highly efficient adsorption material that can be expected to be used to remove methyl orange from dye wastewater.