Two new monoterpenoid indole alkaloids, (2 R, 7 R, 16 R, 20 R, 21S)-12-hydroxypleiocarpine (1) and (2S, 7 R, 16S, 20 R, 21S)-N-methoxycarbonyl-11,12-methylenedioxy-Delta(14,15)-kopsinaline (2), along with six known alkaloids were isolated from the methanol extract of the kernels of Kopsia arborea. Their structures including the absolute configurations were elucidated by HRESIMS, NMR spectroscopy, and quantum computational methods. Their cytotoxicity against two human cancer cell lines were also evaluated.