Dye is an organic substance that seriously threatens the water environment. Using a solvothermal technique, MIL‐100(Fe) and M‐Fe have been synthesized to effectively remove methylene blue (MB) and methyl orange dyes from wastewater. The microstructures of the two products were analyzed using scanning electron microscopy, Fourier transform infrared, Brunauer–Emmett–Teller (BET), thermogravimetric (TG), and X‐ray diffractometer (XPS) test. Optimized the optimal experimental parameters through batch processing experiments, when the pH was 5 and 2, the amount of adsorbent was 50 mg, the temperature was 25°C, and the dye concentration was 30 mg/L, MIL‐100(Fe) and M‐Fe had the highest removal rates of MB, at 98.95% and 94.11%, respectively. Adsorption process was well described by the Freundlich isotherm and pseudo‐second‐order kinetics. After three regeneration experiments, the removal rate was still high. The removal efficiencies of the two adsorbents for MB were similar. However, the regeneration performance of M‐Fe was better. Through the simulation of materials studio, the adsorption energy of the product and MB is −0.93 eV, which is favorable for adsorption. The results show that the two adsorbents can effectively remove MB from wastewater and have broad application prospects.