Nine new alkaloids, (+)-<b>1</b>, (-)-<b>1</b>, <b>2</b>, (+)-<b>3</b>, (-)-<b>3</b>, and <b>4</b>-<b>7</b>, along with five known compounds (<b>8</b>-<b>12</b>), were obtained from the branches and leaves of <i>Elaeocarpus angustifolius</i>. The alkaloids were structurally characterized by NMR and MS data. The absolute configurations of (+)-<b>1</b>, (-)-<b>1</b>, (+)-<b>3</b>, and (-)-<b>3</b> were determined by comparing their experimental and computed electronic circular dichroism spectra. (±)-8,9-Dehydroelaeocarpine (<b>5</b>), (±)-9-epielaeocarpine <i>cis-N</i>-oxide trifluoroacetate (<b>6</b>), and (±)-elaeocarpine trifluoroacetate (<b>9</b>) exerted weak inhibitory activities against butyrylcholinesterase with IC<sub>50</sub> values of 39, 29, and 35 μM, respectively, while that of tacrine, the positive control, was 0.07 ± 0.01 μM. This is the first report of the cholinesterase inhibitory activities of <i>Elaeocarpus</i> alkaloids.