An enantio- and diastereoselective direct vinylogous Mannich reaction of α,α-dicyanoolefins and N-sulfonyl alkylimines has been developed by the catalysis of a new family of bifunctional organocatalysts merging chiral BINOL and 9-amino-9-deoxyepi-cinchona alkaloid skeletons, from which chiral β-, δ- or γ-amino compounds could be efficiently derived.