The psychoactive plant Datura metel appears across a range of traditions in premodern South Asia preserved in texts. Among those traditions is the form of tantric Buddhism (Vajrayāna) located in the yoginī tantras. In Vajrayāna works, the plant is most prominently used in instructions for bringing about one or more of the magical acts (ṣaṭkarman). This paper explores the possibility that datura was consumed for its hallucination-inducing potential by considering how the plant was viewed and used in premodern South Asia through an ethnobotanical approach to relevant texts. I argue that the material potency of the plant as a dangerous poison, well established in Sanskrit medical literature from an early period, gave it a magical potency that made it a favored ingredient in several hostile magic rites (abhicāra) found in the yoginī tantras. I suggest that the line between material and magical is an inappropriate distinction to draw when examining these tantras, and that the most responsible way to approach the use of psychotropic plants in a premodern culture is by examining what actors from that culture said about the plant rather than relying on our existing knowledge of the effect of that plant.