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Caffeine is widely used in the food and pharmaceutical industries. For safety concerns, natural caffeine is preferred over synthetic products despite of its high cost. To explore more economical methods of acquiring natural caffeine, we adopted a microbial fermentation technique to increase the caffeine content of tea leaves. Our studies showed that the caffeine content in tea leaves increased reasonably after treating leaves with microorganisms for a period of time (i.e. orthodox pile-fermentation), and the amount of caffeine content increase varied significantly between black and green teas (27.57% and 86.41%). These results suggested that the change of caffeine content in tea leaves during the pile-fermentation depended not only on the growth and reproduction of microorganisms, but also on the tea composition.