Two new tropolone-bearing sesquiterpenoids (1-2), two new dolabrane-type diterpenoids (3-4) along with eight known compounds as ionone-type sesquiterpenoid (5), oleanane triterpenoid (6), vanillin and its derivative (7-8), neolignan (9), two lignans (10-11), flavanonol glycoside (12) were isolated from whole plants of Croton lauioides Radcl.-Sm. & Govaerts. The structures of all isolated compounds were elucidated by extensive spectral data including 1D, 2D NMR, HR-ESI-MS, and by comparing their NMR data with those of previously reported compounds. The experimental and calculated electronic circular dichroism data were used to determine their absolute configurations. All new compounds (1-4) were evaluated for their anti-inflammatory activity on LPS-induced RAW264.7 macrophages, and cytotoxicity against five human cancer cell lines (HepG2, A-549, MDA-MB-231, HL-60, and SW-480). Compound 2 showed signicant inhibitory activity against NO production with an IC