<jats:title>Abstract</jats:title><jats:p>The roots of the indigenous West African shrub <jats:italic>Cryptolepis sanguinolenta</jats:italic> have proved to be a rich source of indoloquinoline alkaloids. To date, all of the alkaloids isolated have been analogs of indolo[3, 2‐<jats:italic>b</jats:italic>]quinoline. We now wish to report examples of two new indoloquinoline alkaloids which differ in the fusion of the indole and quinoline rings. The first, cryptosanguinolentine, is an angular indolo[3, 2‐<jats:italic>c</jats:italic>]quinoline. The second, cryptotackieine, is a linear indolo[2, 3‐<jats:italic>b</jats:italic>]quinoline system. Both of these families of alkaloids are without precedent from <jats:italic>C. sanguinolenta</jats:italic>. The structures of both were established through the extensive use of inverse‐detected micro nmr methods.