Virgaurol A (1) and B (2), two novel dimeric eremophilanes in whose structures the two asymmetric sesquiterpene units are connected by a C-C bond directly, have been isolated from the roots of Ligularia virgaurea. Their structures were determined by comprehensive spectral analysis. Compound I was evaluated for its in vitro cytotoxic activity against human leukemia (HL-60), human hepatoma (SMMC-7721), and human cervical carcinoma (HeLa) cells.