With optimized conditions in hand, the scope was investigated (Figure ). In general, carbamimidates bearing disubstituted alkenes provided excellent yields (up to 91%) and enantioselectivity (up to 99% ee). Aziridine 2b, which is the (E)-isomer of 2a, was obtained from the corresponding (E)-alkene in 97% ee, suggesting a concerted, stereoretentive mechanism or alternatively, hydrogen atom abstraction followed by rapid radical rebound. Extending the alkyl chain length by one carbon (2c) gave better ee (99% ee), although further extension (2d) surprisingly lowered ee (78% yield, 75% ee). This method was complementary to methods for styrene aziridinations, as 1e provided 2e in only 37% yield and 62% ee. Aziridines containing linear alkyl substituents (2fg) were obtained in excellent yields and ee. The reaction also tolerated a bulky silyl-protected alcohol moiety (2h) or a heteroarene (2i). Increasing the steric bulk proximal to the olefin moiety by installing isopropyl (2j), cyclohexyl (2k), tert-butyl (2l), or adamantyl (2m) groups did not negatively impact either yield or ee. Applicability to complex molecules was highlighted by a lithocholic acid-derived product (2n), obtained as a single diastereomer. The presence of a racemic stereocenter at the secondary alcohol used to form the carbamimidate 1o afforded 2o in a moderate 6.4:1 dr, with a 71% ee of the major stereoisomer. We were pleased to observe both high dr and ee for 2p (> 20:1 dr, 94% ee), highlighting the capability of this method for desymmetrization. The stereochemistries of 2o and 2p were determined by NOESY (see the SI for details).