Metal thiocyanates were some of the first pseudohalide compounds to be discovered and adopt a diverse range of structures. This review describes the structures, properties, and syntheses of the known binary and ternary metal thiocyanates. It provides a categorization of their diverse structures and connects them to the structures of atomic inorganic materials. In addition to this description of characterized binary and ternary thiocyanates, this review summarizes the state of knowledge for all other binary metal thiocyanates. It concludes by highlighting opportunities for future materials development.