<jats:title>Abstract</jats:title><jats:p>Henrycinols A (<jats:bold>1</jats:bold>) and B (<jats:bold>2</jats:bold>), two novel indole alkaloids, together with three known compounds, (+)‐Δ<jats:sup>14</jats:sup>‐vincamine (<jats:bold>3</jats:bold>), (+)‐16‐epi‐Δ<jats:sup>14</jats:sup>‐vincamine (<jats:bold>4</jats:bold>), and (+)‐isoeburnamine (<jats:bold>5</jats:bold>), were isolated from the roots of <jats:italic>Melodinus henryi</jats:italic> <jats:sc>Craib</jats:sc>. Their structures were established on the basis of 1D‐ and 2D‐NMR spectroscopic analysis. The relative configuration of henrycinols A and B was determined by NOESY analysis.