Direct and efficient catalytic reactions with excellent regioselectivity for the preparation of a series of substituted isoindoles, isoquinolines, and imidazoles are reported. Reaction of C6H4 (2-CN) C CR with an array of amines, catalyzed by 10 mol% of [σ: η1: η5- (OCH2)(Me2NCH2) C2B9H9] Ti (NMe2)(1), gives a series of substituted isoindoles in very high yields. In a similar manner, interaction of C6H4 (2-CH2CN) C C-Ph with various ...