Various ethnographic sources have demonstrated the symbolic and ritualistic importance of psychoac- tive plants in Native American societies. The social milieu of these mind- altering plants appears to be ancient. Archaeological evidence during the Tiwanaku empire expansion along the Atacama Desert of Chile, circa 500–1000 A.D., shows the presence of highly decorated snuffing tablets and tubes as grave goods. The preservation of mummified human bodies in the Azapa Valley, northern Chile, provided an opportunity to test the exact nature of the psychoactive plants used in this region. Using gas chroma- tography/mass spectrometry (GC–MS), here we show that ancient Andean populations from northern Chile consumed Banisteriopsis, a vine that contains harmine. This is the first direct archaeological evidence of hallucinogenic and medicinal ethnographic practices. Interestingly enough, this rainforest plant does not grow along the Atacama coast, thus our findings suggest extensive plant trade networks in antiquity as far as the Amazon.