In this study, theaflavin(TF1), theaflavin monogallate(TF2+TF3) and theaflavin digallate(TF4) in tea pigments are isolated and purified with high speed counter current chromatography combined with Sephadex LH-20 and semi-preparative HPLC. With the purified theaflavin, the standard curves have been set up by HPLC for theaflavins quantitation. The results on the accuracy and recovery determination showed that the coefficient of variation of TF1, TF2+TF3, TF4 and total theaflavins range from 2.6’8.5%, 2.0’3.8%, 2.0’3.9% and 2.2’4.1% respectively. Using HPLC quantitation, the relative error of total theaflavins amounts in the standard theaflavins from Sigma company is 3.4%. The total amounts of theaflavins in tea pigments are 20.5%, in which TF1, TF2+TF3 and TF4 are 6.0%, 9.1% and 5.4% respectively. This method is useful to quantify theaflavins and to control the quality of tea pigments, which could promote the studies on their pharmacological effects.