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Previous reports on phytochemicals in green tea (GT) and processed teas mainly focused on more representative compounds such as catechins. Here, we focus on the insignificantly studied non-catechin components in tea extracts, and explore the multivariate correlation between diverse phenolic compounds in tea and the in vitro antioxidant and anticancer effects. Extracts from GT and four types of processed teas were further divided into hydrophilic and hydrophobic fractions, whose phenolic compositions and antioxidant capacities were quantified using HPLC-MS and three antioxidant assays, respectively. For three types of teas, the anticancer effects of their extracts and fractions were assessed using cancer cell lines. The hydrophobic fractions had lower antioxidant capacities than the corresponding hydrophilic fractions, but exhibited superior antiproliferative effects on cancer cells compared with the whole extract and the hydrophilic fraction. Partial least squares-discriminant analysis revealed a strong correlation between the anticancer effects and the theaflavins and flavonols. Therefore, in addition to catechins, the hydrophobic fraction of tea extracts may have beneficial health effects.