In the last decades, the impact of Darwin's legacy has been emphasized in many scientific fields. Nevertheless, there are still lesser-explored aspects of his life as researcher that deserve attention, such as his role as taphonomist. In this context, we highlight here this relevant facet of Darwin's investigations. During his voyage on the H.M.S. Beagle, Darwin collected numerous vertebrate fossils from South America. Particularly, in the Argentine Pampas he recorded information on the paleontology, stratigraphy, and sedimentology of different late Cenozoic fossiliferous sites. He also made observations on the preservation features of bone remains and the mechanisms that favored their fossilization, aspects currently included in the taphonomy field. In this frame, the information published in Geological Observations on South America regarding the fossils from Monte Hermoso and Punta Alta sites and his comments about the “imperfection of the geological record” on the Origin of the Species, are particularly noteworthy as an indicator of his interest in the relationship between the environmental context of preservation and the taphonomic features of bone remains. After 150 years, his scientific work continues to fascinate us. Darwin's keen eye for detail and his curiosity about the history of each fossil, about a century before taphonomy was born as a discipline, can indeed be likened to that of a Crime Scene Investigator (CSI) in some regards, reconstructing the taphonomic histories of both single remains and whole assemblages.