A simple high-yield method for purifying 3,4,5-tri-O-caffeoylquinic acid from sweetpotato leaves (Ipomoea batatas L.) was established. The method consisted of methanol extraction, water-hexane partition, MCI gel CHP20P, and Sephadex LH-20 chromatography. All purification steps required fewer than 3 days, and the yield of purified 3,4,5-tri-O-caffeoylquinic acid was calculated to exceed 76 mg from 100 g of leaf powder. Its recovery was estimated to be more than 66%, and its purity more than 98%.