This chapter discusses the methods used for preparing cluster coordinated nitrosyl ligands, their structural and spectroscopic properties with emphasis on the relationship of terminal and bridging nitrosyls, and their unique reactivity. It also discusses nitride clusters, which are formed using reactions similar to those used for nitrosyl formation and structural, spectroscopic, and reactivity studies. The bonding of the nitrosyl ligand to metal clusters can occur by several modes. A terminal ligand, NO can bind as a linear nitrosyl, which is by far the predominant mode, or as a bent nitrosyl. The primary source of the nitrogen atoms in nitrido clusters is ultimately its monoxide, which is usually coordinated to a transition metal. Such data on these clusters are now available to make a preliminary comparison of the similarities and differences of carbide and nitride ligands. The basic fluxional properties of the carbonyl ligands bound to nitrido clusters are the same as those found for related carbido clusters.