The concept of organocascade catalysis has been harnessed as a strategy for the development of new synthetic reaction methodologies. The merger of orthogonal HOMO and LUMO activation reactivity platforms that utilize two distinct amine catalysts into single multi-cycle reaction sequences has been employed to achieve an array of transformations including alkene diamination, hydroamination, hydro-oxidation, and amino-oxidation as well as reaction-types that had been previously unknown including the formal stereoselective alkylamination and arylamination of olefins.

Furthermore, the extension of the organocascade catalysis concept to the synthesis of a range of high profile natural products has been achieved, including members of the Aromadendrane, Strychnos, Aspidosperma, and Kopsia families. Each synthetic target was selected on the basis of its structural complexity, its established importance in the fields of organic and medicinal chemistry, and its well-recognized status as a ‘benchmark’ compound in total synthesis. In each case, the organocascade-based syntheses are markedly more efficient in comparison to previous enantioselective synthetic routes.