The challenges associated with heat dissipation in high‐power electronic devices used in communication, new energy, and aerospace equipment have spurred an urgent need for high‐performance thermal interface materials (TIMs) to establish efficient heat transfer pathways from the heater (chip) to heat sinks. Recently, emerging 2D materials, such as graphene and boron nitride, renowned for their ultrahigh basal‐plane thermal conductivity and the capacity to facilitate cross‐scale, multi‐morphic structural design, have found widespread use as thermal fillers in the production of high‐performance TIMs. To deepen our understanding of 2D material‐based TIMs, in this review, we focus primarily on graphene and boron nitride‐based TIMs, exploring their structures, properties, and applications. Building on this foundation, we emphasize the developmental history of these TIMs and provide a detailed analysis of critical challenges and potential solutions. Additionally, we briefly introduce the preparation and application of some other novel 2D materials‐based TIMs, aiming to offer constructive guidance for the future development of high‐performance TIMs.This article is protected by copyright. All rights reserved