We determined the phytochemical diversity, including carotenoids, flavonoids, anthocyanins, and phenolic acids, in sweet potatoes ( L.) with distinctive flesh colors (white, orange, and purple) and identified hydrophilic primary metabolites. Carotenoid content was considerably higher in orange-fleshed sweet potatoes, wherein β-carotene was the most plentiful, and anthocyanins were detected only in purple-fleshed sweet potatoes. The levels of phenolic acids and flavonoids were relatively higher in purple-fleshed sweet potatoes than those in the other two varieties. Forty-one primary and 18 secondary metabolite profiles were subjected to multivariate statistical analyses, which fully distinguished among the varieties and separated orange- and purple-fleshed sweet potatoes from white-fleshed sweet potatoes based on the high levels of sugars, sugar alcohols, and secondary metabolites. This is the first study to determine comprehensive metabolic differences among different color-fleshed sweet potatoes and provides useful information for genetic manipulation of sweet potatoes to influence primary and secondary metabolism.