The metal-organic framework MOF-505 particles were synthesized and incorporated into the polyethylene glycol (PEG) matrix to prepare mixed matrix membranes. A series of methods were used to characterize the structure and morphology of MOF-505 particles and membranes. The prepared MOF-505 had a well-developed pore structure, a large number of metal sites for selective adsorption of thiophene and good compatibility with polymer matrix. Accordingly, the desulfurization performance of the membrane was improved effectively. The effects of the content of MOF-505, operating temperature and feed sulfur content on membrane performance were investigated by pervaporation experiments. The membrane with 3 wt% MOF-505 showed the optimal desulfurization performance with a permeation flux of 2.66 kg/(m2.h) and an enrichment sulfur factor of 8.15, which were increased by 158% and 25% versus pristine membrane, respectively.