A new alkaloidal glycoside (1), a new phenylpropanoid glucoside (2), and a new caffeic acid derivative (3) were isolated from the whole plant of Leucosceptrum japonicum, together with eight known phenylethanoid glycosides (4-11), five known flavone glycosides (12-16), three known flavones (17-19), a known phenylpropanoid glucoside (20), a known iridoid glucoside (21), and eight other phenolic or indole compounds (22-29). The structures and stereochemistries of these compounds were elucidated on the basis of the results of spectroscopic analyses.