Selenium is an essential trace element in the human diet and has anti-aging, anti-tumor, and immunity boosting effects. In this study, the effects of selenium on Tartary buckwheat (Fagopyrum tataricum L.) sprouts were investigated. A suitable concentration of selenium had no adverse effects on the growth of Tartary buckwheat seedlings. The soluble sugar, protein, total flavonoid, and total phenol concentrations in the selenium-treated sprouts were higher than those in the untreated control sprouts. Electronic tongue measurements indicated that the taste characteristics, especially the sweetness and umami, of the selenium-treated and untreated groups were significantly different. Sensory analysis showed that selenium-treated Tartary buckwheat sprouts had good acceptability. Selenium-enriched Tartary buckwheat sprouts are a promising product, both in terms of flavor and as a useful source of selenium to increase human dietary intake.