<jats:title>Abstract</jats:title><jats:p>Three new monoterpenoid indole alkaloids, (14<jats:italic>α</jats:italic>,15<jats:italic>α</jats:italic>)‐14,15‐epoxyaspidofractinine (<jats:bold>1</jats:bold>) and maireines A and B (<jats:bold>2</jats:bold> and <jats:bold>3</jats:bold>, resp.), together with 19 known alkaloids, were isolated from the leaves and twigs of <jats:italic>Alstonia mairei.</jats:italic> The structures of the new compounds were elucidated by 1D‐ and 2D‐NMR spectroscopic methods in combination with MS experiments.