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In this chapter, we collect and describe articles published up until April 2018 on the topic of anticancer agents based on two or more different metal centers. Heterometallic compounds have been developed to enhance the anticancer properties of single metallodrugs. The hypothesis that such compounds may have an improved pharmacological profile based on a cooperative and/or synergistic effect of the different metals was first described by Casini and co-workers in 2010. Since then, a number of reports have highlighted the success of this approach. This chapter will focus on examples reported describing not only the anticancer in vitro properties of these compounds, but also providing data on in vivo efficacy trials, as well as on mechanistic studies.

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