Four new 9,10-secosteroids, verrucellols A-D (1-4), together with 12 known derivatives (5-16) were isolated from the gorgonian Verrucella umbraculum collected in the South China Sea. The structures of the new compounds were established by spectroscopic analysis and comparison with reported data. These compounds exhibited significant suppressive effects on CD4+ T lymphocyte cell differentiation in an in vitro bioassay. This is the first report of 9,10-secosteroids exhibiting immunomodulation activity.