Phoneutria Perty, 1833 is considered one of the most toxic spider genera in the world; however, the natural history and biology of these spiders is still largely unexplored. The objective of this study was to determine the natural diet of the medically important species Phoneutria boliviensis (F.O.P.-Cambridge, 1897) based on prey records from Colombia, and supplemented by published records found in electronic databases as well as photographic records from the internet. We found that P. boliviensis is an euryphagous predator with a broad diet made up predominantly of arthropods (orders Araneae, Blattodea, Coleoptera, Hymenoptera, Lepidoptera, Mantodea, Orthoptera, and Phasmatodea) and to a lesser extent of small vertebrates (Gekkonidae, Hylidae, and Sphaerodactylidae). These results support previous evidence suggesting that P. boliviensis is a generalist predator that includes both invertebrates and small vertebrates in its diet.