Two new triterpenoid isomers alpha-neriursate (1) and beta-neriursate (2) have been isolated from the fresh, uncrushed leaves of Nerium oleander and their structures elucidated as 3alpha-acetophenoxy-urs-12-en-28-oic acid and 3beta-acetophenoxy-urs-12-en-28-oic acid, respectively. The structure elucidation is based on spectroscopic methods, including 1D ((1)H NMR, (13)C NMR) and 2D ((1)H-(1)H COSY, NOESY, HMQC, HMBC and J-resolved) NMR data and chemical transformation.