Picrorhiza scrophulariiflora is a traditionally used herb for the treatment of various diseases, including tumors and liver infections. From the roots of Picrorhiza scrophulariiflora, two new secoiridoid glycosides, named picrosecosides I and picrosecosides II have been isolated. Their structures were elucidated on the basis of chemical and spectropic evidences. Two new phenylethanoid glycosides, named scroside H, scroside I, and a new secoiridoid glycoside, named picrogentioside I, have been isolated from the underground parts of Picrorhiza scrophulariiflora. Their structures were elucidated on the basis of spectroscopic evidence. Three new phenylethanoid glycosides, scrosides A-C, and a new iridoid gycoside, picroside IV, have been isolated from the underground parts of Picrorhiza scrophulariiflora, along with 11 known compounds. Their structures were elucidated by 2D NMR spectroscopy and chemical methods.