Nitriles are widely present in various natural products, pharmaceuticals, agrochemicals and dyes. In addition, nitriles are an essential building unit in organic synthesis, which can be readily converted into numerous functional groups. Consequently, the development of new methods for the synthesis of nitriles has gained significant attention in organic synthesis. Over the past few decades, particularly, aryl nitriles were obtained by the cyanation of aryl halides employing metallic/nucleophilic cyano group sources. However, these methods suffer from high catalyst loading and toxic cyano sources. To overcome these problems, various organic cyano group sources have been explored in recent years for the synthesis of nitriles. Among them, cyanamides have attracted significant attention due to their ready availability, ease of handling, and nontoxic and inexpensive nature. In this review, we have summarized the recent developments and applications of cyanamides in the electrophilic cyanation of various nucleophiles.