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An asymmetric organocatalytic aza‐Friedel‐Crafts reaction was developed to give the enantioenriched Δ4‐isoxazoline scaffold bearing a quaternary‐substituted stereogenic centre in good‐to‐excellent yields and enantioselectivity (50–99%, 55–>99% ee). This protocol involves the in situ generated isoxazolium ions in the presence of a chiral phosphoric acid followed by the heteroarene addition through...