The article discusses the role of metals in cancer research, focusing on the development of new anticancer metallodrugs beyond platinum-based compounds. It highlights the importance of organometallic compounds in controlling reactivity and stability in physiological environments, enabling efficient prodrug activation and noncovalent interactions with pharmacological targets. The article also emphasizes the catalytic potential of organometallic compounds in cancer cells, which can be used as selective chemical tools to label targets or enhance biochemical signals. Examples of metallodrugs for "catalysis in cells" are presented, along with other organometallic drug candidates. The selected case studies are discussed in the context of broader challenges in medicinal inorganic chemistry. The article reviews the history and development of platinum-based anticancer drugs, such as cisplatin, and discusses their mechanisms of action, including DNA damage and cell cycle arrest. It also explores the role of other metals, such as ruthenium, iridium, palladium, gold, and titanium, in the development of new anticancer drugs with different modes of action and antiproliferative activities. The article highlights the importance of catalytic organometallic drugs, which can achieve high efficiency at low dosages and overcome cancer cell resistance through novel modes of action. Examples of such drugs include Ru(II) complexes and Au(III) compounds that can induce apoptosis and target specific cancer cells. The article also discusses the use of metal-based compounds in nuclear medicine, including the development of target-specific metal-based radioactive probes for imaging and internal radiotherapy. It highlights the potential of therapeutic radiometals, such as lanthanide isotopes, in treating neuroendocrine tumors and prostate cancers. The article also discusses the emerging field of supramolecular radio-theranostics, which combines therapeutic and diagnostic approaches in cancer treatment. The article concludes by emphasizing the importance of noncovalent interactions in metallodrug reactivity and the need for new chemical guidelines based on a deeper understanding of metallodrug interactions in biological systems. It also highlights the challenges in the field of medicinal inorganic chemistry, including the need to adapt fundamental principles of coordination/organometallic chemistry to better understand and design metallodrugs for cancer treatment.The article discusses the role of metals in cancer research, focusing on the development of new anticancer metallodrugs beyond platinum-based compounds. It highlights the importance of organometallic compounds in controlling reactivity and stability in physiological environments, enabling efficient prodrug activation and noncovalent interactions with pharmacological targets. The article also emphasizes the catalytic potential of organometallic compounds in cancer cells, which can be used as selective chemical tools to label targets or enhance biochemical signals. Examples of metallodrugs for "catalysis in cells" are presented, along with other organometallic drug candidates. The selected case studies are discussed in the context of broader challenges in medicinal inorganic chemistry. The article reviews the history and development of platinum-based anticancer drugs, such as cisplatin, and discusses their mechanisms of action, including DNA damage and cell cycle arrest. It also explores the role of other metals, such as ruthenium, iridium, palladium, gold, and titanium, in the development of new anticancer drugs with different modes of action and antiproliferative activities. The article highlights the importance of catalytic organometallic drugs, which can achieve high efficiency at low dosages and overcome cancer cell resistance through novel modes of action. Examples of such drugs include Ru(II) complexes and Au(III) compounds that can induce apoptosis and target specific cancer cells. The article also discusses the use of metal-based compounds in nuclear medicine, including the development of target-specific metal-based radioactive probes for imaging and internal radiotherapy. It highlights the potential of therapeutic radiometals, such as lanthanide isotopes, in treating neuroendocrine tumors and prostate cancers. The article also discusses the emerging field of supramolecular radio-theranostics, which combines therapeutic and diagnostic approaches in cancer treatment. The article concludes by emphasizing the importance of noncovalent interactions in metallodrug reactivity and the need for new chemical guidelines based on a deeper understanding of metallodrug interactions in biological systems. It also highlights the challenges in the field of medicinal inorganic chemistry, including the need to adapt fundamental principles of coordination/organometallic chemistry to better understand and design metallodrugs for cancer treatment.