Mild Control: Selective cyclization of aminocyclopropanes on the N1 or C3 positions of indole was achieved by tuning the catalyst and solvent. The new strategy was applied to the formal synthesis of aspidospermidine and the total synthesis of goniomitine in 13 steps and 11% overall yield. The first studies on the bioactivity of goniomitine demonstrated significant cytotoxicity against several tumor cell lines (IC50: 150-400 nM).