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Imidazolium-based zinc-containing ionic liquids (ILs), [1-R-3-R′-imidazolium]alkylsulfate-ZnCl2 (R and R′ = H or alkyl), were highly effective for the denitrogenation of a model oil containing quinoline, indole, or acridine in n-heptane. Fast atom bombardment (FAB)−mass spectra and a computational study imply that the interaction of 1-ethyl-3-methylimidazolium ethylsulfate ([EMIm]EtSO4) with ZnCl2 produces Zn-containing ILs, presumably [EMIm]ZnCl2(EtSO4) and [EMIm]ZnCl(EtSO4)2 as the major ionic species. The interaction of EtSO4 − and ZnCl2(EtSO4)− with a heterocyclic N compound was theoretically investigated. The zinc-containing IL, [EMIm]ZnCl2(EtSO4), used for the extraction of quinoline was successfully regenerated by employing diethyl ether as a back extractant.