We studied the synthesis, characterization clarification, and dye adsorption ability of chromium-based metalorganic framework (Materials Institute Lavoisier: MIL-101(Cr)). MIL-101(Cr) with 1 : 1 molar ratio of metal to ligand was ultrasound-assisted green synthesized in a DMF-free way and its adsorption capacity for pollutant remediation was studied. Several analyses were applied to clarify the characterization of materials, including TGA, SEM, XRD, FTIR, BET, and Zeta potential. Direct Red 80 (DR80) and Acid Blue 92 (AB92) were used to make model dye bearing wastewater. Response surface methodology (RSM) historical modeling was applied to the data to achieve an accurate model of the experiment. Adsorption kinetics and isotherms models were fully studied. The powerful adsorbent was the MIL- 101(Cr) with the M/L=1 : 1, which represented the high specific surface area (SSA) of 2,420m2/g and surface charge of +27.2mV. The maximum adsorption capacity was obtained 227mg/g for DR80 and 185mg/g for AB92. With an eye to the real-world application, the synthesized adsorbent well operated by removing dyes from the wastewater and high reusability after four cycles.