This research was to study the adsorptive desulfurization of DBT and 4,6-DMDBT with sulfur 150 ppm in n-octane as model oil. The adsorption experiments were performed in a fixed-bed flowing system with flow rate of 1 mL/min at ambient temperature. For adsorptive desulfurization over three unmodified adsorbents including activated alumina, activated carbon and Na-Y zeolite, the breakthrough and saturation capacities were calculated by the breakthrough curve and the adsorption capacities followed the order: Na-Y zeolite > activated carbon > activated alumina. Thus, activated carbon and Na-Y zeolite were selected to study the surface modification for enhanced adsorption performance. Activated carbon was impregnated with Cu and Ni of 5, 10, 15, 20 and 30 %wt. The results indicated that 10 %wt Cu/AC and 10 %wt Ni/AC adsorbents showed a good adsorption of both sulfur compounds because impregnation of metal could improve the adsorptive sites. In addition, Na-Y zeolite was also modified to Cu-Y zeolite and Ni-Y zeolite with ion-exchange method. For adsorption of DBT and 4,6-DMDBT, Cu-Y zeolite and Ni-Y zeolite had higher adsorption capacities than NaY-zeolite because Cu and Ni ions could form a π–complexation bond with sulfur compounds. The adsorption capacities of both sulfur compounds followed the order: Cu-Y zeolite ~ Ni-Y zeolite > 10 %wt Cu/AC ~ 10 %wt Ni/AC adsorbents. For adsorption 4,6-DMDBT on Cu-Y zeolite, the adsorption capacities increased with decreasing flowrate and increasing temperature.