Phyllobilins are a group of chlorophyll‐derived bilin‐type linear tetrapyrroles, generated in the process of chlorophyll breakdown. Since the first phyllobilin was isolated and characterized in 1991, more and more structures of these chlorophyll catabolites were identified alongside the biochemical players involved in chlorophyll breakdown. In the meantime, phyllobilins are known to occur in a large natural structural variety, and new modifications are still being discovered. Phyllobilins have been regarded as products of chlorophyll detoxification for a very long time, hence they have been completely overlooked as a natural product class in terms of their biological role or pharmacological activity. A change of this paradigm, however, is long overdue. Here, we review the current knowledge of the pharmacological activities of phyllobilins and give an overview of the diverse structural modifications, laying the groundwork for analyzing their role(s) as active components in medicinal plants.