Publisher Summary This chapter covers methods by which a nitrile group is introduced into another compound and those in which the nitrile group is formed in situ by the elimination of elements or groups. The chapter mentions a method of converting a reactive methyl group into a nitrile. The chapter describes methods of nitrile synthesis , which are true substitution reactions, such as the reaction of an organic halide with a metal cyanide, and also those reactions , which superficially appear to be substitutions , but , which proceed by a different mechanism, for example, by acid-nitrile exchange. The chapter is concerned either with reactions in which the addition of hydrogen cyanide (HCN) to multiple bonds results in the formation of a nitrile, directly, or on subsequent reaction or rearrangement. While the addition of HCN to an alkene or alkyne remains an important industrial process, there have been few innovations of value to laboratory scale nitrile synthesis.