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Gold(I) NHC complexes containing different phosphanes as secondary ligands were shown to trigger strong cytotoxic effects in cancer cells, and their effective uptake into the cells was quantified by atomic absorption spectroscopy. Moreover, the new compounds strongly inhibited the activity of the seleno\u2010enzyme thioredoxin reductase (TrxR) and of the zinc\u2010finger enzyme poly(ADP\u2010ribose) polymerase\u20051 (PARP\u20101). In the case of TrxR inhibition, their activity depended clearly on the size of the alkyl\/aryl residues of phosphorus atoms. Density functional theory (DFT) calculations showed that the Au\uf8ffP bond of the triphenylphosphane complex [Au<jats:sup>I<\/jats:sup>(NHC)(PPh<jats:sub>3<\/jats:sub>)]I had a lower bond dissociation energy compared to trialkylphosphane complexes [Au<jats:sup>I<\/jats:sup>(NHC)(PR<jats:sub>3<\/jats:sub>)]I, indicating a higher kinetic reactivity of this particular compound. 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