Metal cluster molecules are discrete compounds containing multiple metal atoms held together by metal–metal and metal–ligand bonding. They serve as excellent candidates for catalysts, biosensors, and even for drug development. Developing atomic-level molecular editing methods for such metal clusters remains an important challenge and represents a promising strategy for expanding their structural and functional diversity. Such approaches can enable structure-specific properties, high near-infrared (NIR) photoluminescence quantum yields, and unique reactivities and electronic structures.