A novel composite adsorbent, PTA@(Zn, Ni, Cu)-BTC, was prepared by (Zn, Ni, Cu)-BTC doped with different amounts of phosphotungstic acid (PTA) using an impregnation method. Apparatus like nitrogen adsorption desorption, X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared (FT-IR), inductively coupled plasma optical emission spectroscopy (ICP-OES), and NH3-temperature programmed desorption (NH3-TPD) are employed to characterize our obtained adsorbents. The adsorption properties of as-prepared adsorbents for the dibenzothiophene (DBT) were evaluated by means of fixed-bed breakthrough experiments. Unlike conventional MOFs (metal organic frameworks), the PTA@(Zn, Ni, Cu)-BTC exhibited high DBT selectivity adsorption performs with a superior uptake capacity compared with those previously reported in the literatures. Additionally, PTA@(Zn, Ni, Cu)-BTC showed a remarkable stability in the presence of benzene and acetone, maintaining about 95% initial uptake capacity after eight regeneration procedures. PTA@(Zn, Ni, Cu)-BTC is confirmed to be a hopeful material for DBT capture toward deep desulfurization.