Abstract: Stable and radioactive metal ions possess attractive properties for biomedical imaging and therapy. Our lab applies a cross-disciplinary approach that combines physical inorganic chemistry, coordination chemistry, chemical biology and preclinical imaging to transform aqua ions into tools for non-invasive diagnostic imaging, optical probes for image-guided surgical resection and targeted radiotherapy of cancers. I will discuss 1) strategies to stabilize hydrolytic, radioactive metal ions as mononuclear coordination complexes for targeted imaging and 2) photochemical/thermally activated isotope capture and release systems for the synthesis of radiopharmaceuticals.