Triple selectivity: Highly substituted indenylamines can be obtained with high enantioselectivity by formal [3+2] additions of aryl ketimines with internal alkynes. These rhodium(I)-catalyzed processes proceed by selective C-H activation of one of the two arene substituents, regioselective carbometalation of the alkyne, and enantioselective addition across the imine. Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.