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A series of novel aqueous ionic liquids (NMP-FeCl3-nH2O) were prepared and the effects of water in the aqueous ionic liquids on desulfurization rate and selectivity of simulated FCC gasoline were investigated. The results showed that adding a small amount of water into the ionic liquid NMP-FeCl3 could effectively improve the desulfurization rate and selectivity, and the optimal amount of water was equal to 5%―10% of NMP. Finally, the possible desulfurization mechanism activated by a small amount of water was proposed.