The data presented in this paper provide direct microbotanical evidence concerning the early use of potato (Solanum tuberosum) within its botanical locus of origin in the high south-central Andes. The data derive from Jiskairumoko, an early village site in the western Titicaca Basin dating to the Late Archaic to Early Formative periods (∼3,400 cal y BC to 1,600 cal y BC). Because the site reflects the transition to sedentism and food production, these data may relate to potato domestication and early cultivation. Of 141 starch microremains recovered from 14 groundstone tools from Jiskairumoko, 50 are identified as consistent with cultivated or domesticated potato, based on reference to published materials and a study of wild and cultivated potato starch morphology. Along with macro- and microbotanical evidence for chenopod consumption and grinding tool data reflecting intensive use of this technology throughout site occupation, the microbotanical data reported here suggest the intensive exploitation, if not cultivation, of plant resources at Jiskairumoko. Elucidating the details of the trajectory of potato domestication is necessary for an overall understanding of the development of highland Andean agriculture, as this crop is central to the autochthonous agricultural suite. A paucity of direct botanical evidence, however, has hindered research efforts. The results of the modern and archaeological starch analyses presented here underscore the utility of this method in addressing questions related to the timing, mode, and context of potato origins.