Carbonyl chalcogenide metal coordination polymers have drawn much attention in recent decades owing to their fascinating structures, variable bonding modes, and potential applications in material science. While most polymers were constructed by transition metal carbonyls that were further linked by chalcogen atoms or chalcogen-containing ligands, some polymers were built from predesigned chalcogen-containing metal carbonyl clusters that were bridged by organic or inorganic ligands. The significant interactions between electronegative chalcogens and electropositive metal carbonyls along with variable non-classical weak interactions within the frameworks were found to enhance the stability of the resultant supramolecules and polymers under ambient conditions. In addition to some representative metal carbonyl chalcogenide polymers, this chapter will mainly cover carbonyl chalcogenide cluster-based supramolecules and polymers from groups 6 to 8 metals in terms of syntheses, structural features, and their potential applications in the fields of semiconductors, photodegradation, magnetism, catalysis, and adsorption/desorption.