A high-performance Ni/ZnO adsorbent was prepared by homogeneous precipitation using urea hydrolysis and characterized by N adsorption-desorption, X-ray diffraction (XRD), and scanning electron microscope (SEM). The adsorbent was applied to the deep desulfurization of gasoline and showed a high breakthrough sulfur capacity and a remarkably high volume hourly space velocity. The effects of coexisting olefins in gasoline as well as adsorptive conditions on the adsorptive performance were examined. It was found that olefins in gasoline had a slightly inhibiting effect on the desulfurization performance of the adsorbent. The optimum conditions were 673 K, 1.0 Mpa with a volume hourly space velocity of 60 h . Under the optimum conditions, ultralow sulfur gasoline could be produced and the breakthrough sulfur capacity of the adsorbent was 360 mg-s/g-sorb for the model gasoline.