Fifteen new labdane-type diterpenoids, sublyratins A-O (1-15), along with four known analogues (16-19) were isolated from the aerial parts of Croton sublyratus. Their structural assignments were challenging due to the stereoisomeric features evident and were achieved by analyzing comprehensively the spectroscopic data and electronic circular dichroism spectra and using X-ray crystallographic analysis. Compounds 9 and 16-18 displayed cytotoxic activity against the HL-60 cell line with IC50 values of 1.5-2.8 μM.