Although great progress has been made in the synthesis of metal nanoparticles, good repeatability and accurate predictability are still difficult to achieve. This difficulty can be attributed to the synthetic method based primarily on observation and subjective experience, and the role of many surfactants remains unclear. It should be noted that surfactants play an important role in the synthetic process. Understanding their function and mechanism in the synthetic process is a prerequisite for the rational design of nanocatalysts with ideal morphology and performance. In this review article, the function of surfactants is introduced first, and then the mechanism of action of surfactants in controlling the morphology of nanoparticles is discussed according to the types of surfactants, and the promoting and sealing effects of surfactants on the crystal surface is revealed. The relationship between surfactants and the morphology structure of nanoparticles is studied. The removal methods of surfactants are discussed, and the existing problems in the current development strategy are summarized. Finally, the application of surfactants in controlling the morphology of metal nanocrystals is prospected. It is hoped that the review can open up new avenues for the synthesis of nanocrystals.