A panel of [AuIII(C⁁N)(R2NCS2)]+ (HC⁁N = 2-phenylpyridine) complexes displayed significant deubiquitinases (DUBs) inhibitory activity; one of these complexes showed selective in vitro cytotoxicity towards breast cancer cells correlated to high cellular uptake of gold, and induced cell-cycle arrest, apoptosis, and anti-angiogenic property that could be related to DUB inhibitory activity.