MIL-53(Cr) is one of the important metal-organic frameworks owing to its unique structural properties. Generally, MIL-53(Cr) was prepared with the addition of hydrogen fluoride and a large amount of solvent at 220 degrees C for 72 h. In this work, we report that MIL-53(Cr) can be synthesized in a shorter crystallization time (48 h) by a facile and green route and this route is demonstrated to be scalable. The optimized material (MIL-53(Cr)-G) possessed a high surface area and rich porosity similar to that of conventional MIL-53(CO. Differently, it displayed a triangular prism morphology with a high crystal plane ratio of (110)/(200) and a relatively large crystal size. Meanwhile, a new time-saving and energy-efficient method was developed to purify the as-synthesized MIL-53(Cr). In addition, MIL-53(Cr)-G as an adsorbent exhibited excellent adsorption desulfurization performance (86.4 mg S/g) in the removal of dibenzothiophene from model oil. After the optimization of the regeneration method, such an outstanding adsorption performance can still be kept after 5 runs.