MIL-53(Fe) as a three-dimensional MIL was prepared with different precursors-to-solvent ratios and denoted as MIL53B and MIL53C. All as-synthesized samples were modified using 3-amino propyl trimethoxy silane (organosilane) for synthesizing MIL53B/NH2(0.10), MIL53B/NH2(0.20), MIL53B/NH2(0.30), MIL53C/NH2(0.10), MIL53C/NH2(0.20), and MIL53C/NH2(0.30), respectively. The XRD, SEM, EDS, and FTIR techniques were used to characterize materials. The adsorption ability of the materials for the adsorption of dye (Direct Red 23) was studied. The effect of operational parameters was evaluated. The kinetics and isotherm of pollutant removal obeyed pseudo-second-order kinetic and the Langmuir models, respectively. The row and modified MIL53B indicated the adsorption capacity of 1,375 and 4,989 mg/g, respectively. The high pollutant removal ability and fast adsorption rate ascertain that the modified MIL53 could be considered as a dye adsorbent and potentially other organic molecules with similar structures from contaminated water.