Treatment of various phenylsulfoximines with nBuLi (1 equiv.) at -78°C in THF resulted in single ortho-lithiations and gave the corresponding o-lithiosulfoximines. According to NMR spectroscopy, the o-lithiosulfoximines are generally stable at 0°C. The o-lithiosulfoximines were efficiently trapped through deuteration, alkylation, silylation, and phosphanylation. Treatment of cyclic phenylsulfoximines also containing H atoms at their α-positions with nBuLi (1 equiv.) at -78°C furnished the o-lithiosulfoximines with high selectivity, whereas similar treatment at -50°C to room temperature yielded the corresponding α-lithiosulfoximines. At elevated temperatures, o-lithiosulfoximines also possessing α-H atoms underwent quantitative o,α-transmetalation to afford the corresponding α-lithiosulfoximines. Treatment of α,α-disubstituted cyclic and α,α,α-trisubstituted acyclic phenylsulf-

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