LAUSR

The Rauhut‐Currier reaction generally employs α,β‐unsaturated carbonyl compounds and nitroalkenes as the substrates. Here we develop an enantioselective formal [4+2] annulation reaction, which is initiated by an intermolecular cross Rauhut‐Currier reaction between electron‐deficient ortho‐formyl‐styrenes and 2‐benzoyl‐acrylonitriles catalyzed by an L‐phenylglycine‐derived phosphine, followed by a cascade aldol/acyl transfer/elimination process. A series of enantioenriched dialin frameworks with an unusual exo‐double bond are furnished in fair to good yields with moderate to excellent enantioselectivity, and the architectures with higher molecular complexity can be constructed via simple transformations.