Four new vibsane-type diterpenoids, vibsanol I (1), 15-hydroperoxyvibsanol A (2), 14-hydroperoxyvibsanol B (3), 15-O-methylvibsanin U (4), and a new natural product, 5,6-dihydrovibsanin B (5), as well as six known analogues, were isolated from the twigs and leaves of Viburnum odoratissimum. Their structures were elucidated by spectroscopic analyses and chemical derivatization method. All compounds showed different levels of cytotoxicity against five cell lines (HL-60, A-549, SMMC-7721, MCF-7, and SW480). Remarkably, 14,18-O-diacetyl-15-O-methylvibsanin U (4a) showed significant cytotoxicity against HL-60, A-549, SMMC-7721, MCF-7, and SW480, with IC50 values of 0.15 +/- 0.01, 0.69 +/- 0.01, 0.41 +/- 0.02, 0.75 +/- 0.03, and 0.48 +/- 0.03m, respectively. In addition, vibsanin K (10) was identified as a HSP90 inhibitor with an IC50 value of 19.16m.