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The constitutive activation of the PI3K/mTOR pathway in cancer cells has been validated by epidemiological and experimental studies as an essential step towards the initiation and maintenance of human tumors. A number of intracellular components of this pathway have been targeted for anti-cancer drug discovery activities leading to the current panoply of clinical trials of PI3K/mTOR pathway modulators. The progress in the identification and development of early polypharmacology-based inhibitors that concomitantly target PI3K and mTOR is presented and discussed in this chapter.

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