AgCeY-n zeolites with different Si/Al ratios n (n = 3.0, 4.8, and 5.3) were successfully prepared and characterized by XRD, BET analysis, SEM, IR spectroscopy, XPS, FTIR spectroscopy, and ICP analysis. The effects of the Si/Al ratio on the adsorptive desulfurization properties of the adsorbents were evaluated. The results showed that AgCeY-5.3 exhibited the best sulfur removal capacity and selectivity. The capacity for sulfur removal onto AgCeY-n decreased in the order AgCeY-5.3 > AgCeY-4.8 > AgCeY-3.0 for a model oil comprising thiophene (TP) and benzothiophene (BT), along with certain amounts of toluene or cyclohexene. The adsorption affinity of the sulfur compounds was in the order BT > TP. In addition, the inhibition effects on the AgCeY-n zeolites for sulfur removal were in the order cyclohexene > toluene. The removal of organic sulfur compounds onto AgCeY-n was mainly by pi-electronic and direct coordination (S-M) interaction.