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Herein we present a library of fully characterized β‐diketonate and β‐ketoiminate compounds that are functionalized with a ferrocenyl moiety. Their cytotoxic potential has been determined by screening against human breast adenocarcinomas (MCF‐7 and MDA‐MB‐231), human colorectal carcinoma  p53  wild type (HCT116  p53   +/+  ) and normal human prostate (PNT2) cell lines. The ferrocenyl β‐diketonate compounds are more than 18 times more cytotoxic than the ferrocenyl β‐ketoiminate analogues. Against MCF‐7, compounds functionalized at the  meta  position are up to nine times more cytotoxic than when functionalized at the  para  position. The ferrocenyl β‐diketonate compounds have increased selectivity towards MCF‐7 and MDA‐MB‐231, with several complexes having selectivity index (SI) values that are more than nine times (MCF‐7) and more than six times (MDA‐MB‐231) that of carboplatin. The stability of these compounds in dimethyl sulfoxide (DMSO) and dimethylformamide (DMF) has been assessed by NMR spectroscopy and mass spectrometry studies, and the compounds show no oxidation of the iron center from Fe II  to Fe III . Cytotoxicity screening was performed in both DMSO and DMF, with no significant differences observedin their potency.

β‐Diketonate versus β‐Ketoiminate: The Importance of a Ferrocenyl Moiety in Improving the Anticancer Potency