The leaves of Catharanthus roseus (L.) G. Don. is the source of pharmaceutically valuable terpenoid indole alkaloids (TIAs) such as anticancer drugs vinblastine and vincristine. In particular, vindoline and catharanthine are harvested from leaves and used for the semisynthetic production of vinblastine and vincristine. Because of this, catharanthine and vindoline can be used to screen for high-yielding TIA cultivars. In this study we determined the TIAs concentrations of the leaves of 77 different cultivars of C. roseus. Serpentine contents among the 77 germplasms showed highest concentration in Vinca Pacifica Apricot (519.0 μg/g DW) while vindoline (2082.3 μg/g DW) and catharnathine (2903.4 μg/g DW) were the highest in Vinca Pacifica Peach. Additionally, Vinca Pacifica Peach (5041.0 μg/g DW) had the highest total TIAs concentrations. The 77 germplasms were classified into seven types according to their characteristic: Vinca Sunshower, Vinca Sunstorm, Vinca Cooler, Vinca Pacifica, Vinca Mediterranean, Vinca Titan, Vinca Stardust. Among the seven types, Vinca Sunstorm (3120.4 μg/g DW) had the highest average total TIAs concentrations in C. roseus leaves. This study indicates that cultivars of Vinca Sunstorm type have the potential to be industrial important cultivars for the production of vinblastine and vincristine.