Optically pure hetero‐organic catalysts that bear a hydroxyl moiety, a stereogenic sulfinyl group, and a chiral amine moiety, are highly efficient in the asymmetric aziridination of unsaturated aldehydes and lead to the desired chiral products in high yields (up to 93 %) with enantiomeric excess values up to 92 %. The influence of the stereogenic centers at the sulfinyl sulfur atom and in the amine moiety on the stereochemical outcome of the title reaction is discussed.
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