Abstract: Accumulated heat is the primary problem that needs to be solved in current electronic products. There is an urgent need for designing innovative high-performance thermal interface materials (TIMs) with excellent heat dissipation performance. Based on the development status of TIMs, graphene paper-based TIMs that are ultrathin thickness and have high through-plane thermal conductivity show great potential. From this perspective, we introduce four types of graphene paper (including graphene/polymer composite papers, graphene/metal composite papers, graphene/ceramic composite paper, and graphene/carbon composite paper) and vertically aligned graphene paper as TIMs. Based on the applications of these TIMs, their advantages and limitations are discussed. Finally further research prospects are proposed to promote the practical applications of graphene paper-based TIMs.