Phytochemical investigation of the 50% ethanol eluate fraction of macroporous resin for the flower of Datura metel L. led to the isolation of a new compound named yangjinhualine A (1) and five known megastigmane sesquiterpenes through repeated silica gel and ODS column chromatography and semipreparative HPLC. The structures of these compounds were determined by spectroscopic methods, including 2D-NMR, ESI-MS, and HR-ESI-MS spectrometry as well as by comparison with published data. Five known megastigmane sesquiterpenes were also isolated from D. metel L. for the first time.