Two-dimensional (2D) materials have attracted considerable attention because of their novel and tunable electronic, optical, ferromagnetic, and chemical properties. Compared to mechanical exfoliation and chemical vapor deposition, polymer-assisted deposition (PAD) is more suitable for mass production of 2D materials owing to its good reproducibility and reliability. In this review, we summarize the recent development of PAD on syntheses of 2D materials. First, we introduce principles and processing steps of PAD. Second, 2D materials, including graphene, MoS2, and MoS2/glassy-graphene heterostructures, are presented to illustrate the power of PAD and provide readers with the opportunity to assess the method. Last, we discuss the future prospects and challenges in this research field. This review provides a novel technique for preparing 2D layered materials and may inspire new applications of 2D layered materials.