Three new alkaloids, namely, 4,6-dien-3-oxo-N-demethylconanine (pubescine), 1,4-dien-3-oxo-N-demethylconanine (norholadiene) and 3-dimethylamino-5-en-12 alpha-hydroxyconanin (pubescimine), have been isolated from the bark of Holarrhena pubescens and their structures elucidated through exhaustive 1D and 2D NMR (COSY-45, NOESY, J-resolved and HMQC).