<jats:title>Abstract</jats:title><jats:p>A new indole alkaloid, streptomycindole (<jats:bold>1</jats:bold>), and a known related compound, <jats:italic>N</jats:italic>‐phenylacetyl‐<jats:sc>L</jats:sc>‐tryptophan (<jats:bold>2</jats:bold>), have been isolated from <jats:italic>Streptomyces</jats:italic> sp<jats:italic>.</jats:italic> DA22, associated with South China Sea sponge <jats:italic>Craniella australiensis.</jats:italic> Their structures were established on the basis of a combination of mass spectrometry, <jats:sup>1</jats:sup>H‐ and <jats:sup>13</jats:sup>C‐NMR spectroscopic analyses, and chemical methods.