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A family of stable anticancer gold(III)-based therapeutic complexes containing cyclometalated triphenylphosphine sulfide ligands have been prepared. The anticancer properties of the newly developed complexes [AuCl2κ2-2-C6H4P(S)Ph2] (1), [Au(κ2-S2CNEt2)κ2-2-C6H4P(S)Ph2]PF6 (2), [AuCl(dppe)κC-2-C6H4P(S)Ph2]Cl (3), and [Au(dppe)κ2-2-C6H4P(S)Ph2][PF6]2 (4) were investigated toward five human cancer cell lines [cervical (HeLa), lung (A549), prostate (PC3), fibrosarcoma (HT108, and breast (MDA-MB-231)]. In vitro cytotoxicity studies reveale