Polyeptoids are a promising class of polypeptide mimetic biopolymers based on N-substituted glycine backbones. Because of the high designability of their side chains, polypeptoids have a wide range of applications in surface antifouling, biosensing, drug delivery, and stimuli-responsive materials. To better control the structures and properties of polypeptoids, it is necessary to understand different methods for polypeptoid synthesis. This review paper summarized and discussed the main synthesis methods of polypeptoids: the solid-phase submonomer synthesis method, ring-opening polymerization method and Ugi reaction method.