To separate and purify tea polyphenols and caf­feine from discarded green tea crude extract with macropo­rous adsorption resins (MARs), the adsorption properties of twenty kinds of MARs are systematically evaluated. The results show that GS-18 has higher separation efficiency than other MARs, and the experimental data fit best to the pseudo-second-order kinetic model. And adsorption iso­therms and thermodynamics of tea polyphenols and caf­feine on GS-18 are investigated. The separation parameters of tea polyphenols and caffeine from discarded green tea crude extract are optimized according to dynamic adsorp­tion/desorption experiments with the column packed with GS-18. Through only one cycle treatment, the content of tea polyphenols increases 3.0-fold from 20 to 60 % with a recovery yield of 91 % and that of caffeine increases 3.1- fold from 7 to 22 % with a recovery yield of 98 %. The results demonstrate that the method of MARs will provide useful help for the development of large-scale separation of tea polyphenols and caffeine from discarded green tea in industry.