The present work is dedicated to the development and application of oxidative palladium(II)-catalyzed carbocyclizations. A general procedure for an aerobic palladium(II)-catalyzed endo cyclization of indole derivatives is presented. Further application of this new methodology in the synthesis of C-2 alkenylated indoles in diastereomerically pure form is also reported. The other methodologies involves hydroxy-directed diastereotopic group selection of prochiral bis(homoallylic) alcohols and enantioselective Fujiwara–Moritani cyclizations. In addition to this, the book also details on the indole directed aerobic dehydrogenation of cyclohexenes.