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1,3‐Disubstituted N‐aryl‐2H‐isoindoles have been synthesized by a cascade reaction of divinyl ethers, which are derived from easily available 4‐bromoisocoumarins, with substituted anilines in HFIP. This cascade reaction consists of a ring‐opening step through addition‐elimination mechanism and the following 5‐exo‐tet type ring‐closing step via the intramolecular nucleophilic substitution reaction...