Two new Daphniphyllum alkaloids, 4,21-deacetyl-deoxyyuzurimine (1) and macropodumine L (2), together with the two known related alkaloids, have been isolated from the bark of Daphniphyllum macropodum Miq. The structures of the new compounds were elucidated on the basis of the detailed analysis of spectroscopic data, chemical method, and by comparison of the spectroscopic data with those of known compounds. Compounds 2 and 4 exhibited weak cytotoxicity against human carcinoma cell lines SMMC-7721 and HO-8910.