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Graphical abstract: <br>Display Omitted<br>Highlights: ► <b>Ligularia achyrotricha</b> is a traditional Tibetan medicine. ► Ligulachyroine A, a new alkaloid was isolated from the roots of <b>L. achyrotricha</b>. ► Eleven known compounds were also isolated from this species. ► Ligulachyroine A exhibited moderate activity against HL-60 and SMMC-7721 cells.<br><b>Ligularia achyrotricha</b> (Diels) Ling has been used as a traditional Tibetan herbal medicine. Ligulachyroine A (<b>1</b>), a new twelve-membered macrocyclic pyrrolizidine alkaloid with a ketonic group located at C-3 and an hydroxy group linked at C-8, was isolated from the roots of <b>L</b>. <b>achyrotricha</b>. It is particularly noteworthy that the structure of <b>1</b> rarely appears in any other naturally occurring twelve-membered macrocyclic pyrrolizidine alkaloid reported to date. Three known lignans (<b>2</b>-<b>4</b>) and eight known coniferyl and sinapyl alcohol derivatives (<b>5</b>-<b>12</b>) were also obtained in this species. Their structures were elucidated through a careful analysis of their IR, MS, and NMR spectra. Compound <b>1</b> exhibited moderate activity against HL-60 and SMMC-7721 cells.