Abstract: Because of their uniquely high thermal and chemical stabilities, carboranes have become a subject of study with high interest in the chemistry of supramolecules, catalysts and radiopharmaceuticals. In recent years, the role of carboranes in nuclear medicinal chemistry has been diversified, from the traditional use in boron neutron capture therapy (BNCT), to the clinical applications in molecular radioimaging and therapy. This paper provides an overview of the synthesis and characterization of carboranes and their applications in nuclear medicinal chemistry, with highlights of recent key advancements in the research areas of BNCT and radioimaging.