In order to utilize waste tea flowers (Camellia sinensis L O Kuntze) and develop an industrialized way to refine tea flower polyphenols, a novel method for obtaining high purity of tea flower polyphenols by various ethanol concentration gradient elution was established based on the previous technology of “ultra-filtration-resin absorption-ethanol elute extraction of tea flower polyphenols”. The results showed that an average content as high as 92.25% of refined tea flower polyphenols could be collected by gradient elution of 10%, 20%, 30% and 40% ethanol elute followed, whereas single elution of 70% ethanol elute only led to 84.32% content of tea flower polyphenols. Therefore, catechins in various eluant components were effectively separated. There was also a good correlation between their purity and scavenging efficiency of ?OH and DPPH?, both of which were higher than that of the crude extracts. Ethanol (20%) elution led to the highest EGCG content of 67.39%, and effectively removed theine in the final products which may directly used as antioxidants.