The whole plant ethanolic extract of Solenanthus lanatus was used for the isolation of acetylcholinesterase inhibitors. A new pyrrolizidine alkaloid, 7-O-angeloylechinatine N-oxide, 1, was isolated together with three known compounds of the same class (3-O-acetylheliosupine N-oxide, 2, heliosupine N-oxide, 3, and heliosupine, 4), by bioassay-guided approach. Their structures were elucidated by spectroscopic methods. All the isolated compounds showed inhibition activity against the AChE, with IC50 0.53-0.60mM.