The field of aminocatalysis, defined as the aptitude of a primary or secondary amine to catalyze reactions using carbonyls such as ketones or aldehydes, has rapidly evolved in the last ten years. These researches have led to considerable efforts in new catalysts developments. Unfortunately, most of the newly designed organocatalysts remain specific, as for the over-studied Michael addition to nitroolefins. Thus, the development of new catalysts with a broad range of applicability would be of great interest. During this phD, we discovered a new family of catalysts called Aminal PYrrolidine (APY). Based on a maximized steric hindrance and modularity of the catalysts, they afford excellent enantioselectivities on a broad range of different reactions. Furthermore, those catalysts were further applied to new highly challenging reactions. They allowed us to discover unprecedented reactions by applying new Michael acceptors and donors. In addition, by combining different modes of catalytic activation (organometallic and enamine) in a single-pot, a new approach for the generation of complex molecules has been explored.