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Abstract: Endogenous β‐carbolines, such as harmane, are known to occur in mammalian species including humans. Radioligand binding studies have revealed that certain β‐carbolines display high affinity for both I₁ and I₂ imidazoline‐binding sites (IBS). Functional studies have shown that the β‐carboline harmane elicits many characteristics expected of an endogenous ligand IBS. This article discusses the evidence relating to β‐carbolines as endogenous ligands and presents a case for harmane and related compounds as endogenous ligands for IBS.