The rapid increase of the packaging integration and power density of devices in electronics leads to urgent demands for high-performance thermal interface materials (TIMs) to efficiently solve the accompanying thermal management problem. Although various highly thermally conductive materials (such as graphene, carbon nanotube, and boron nitride nanosheet) combined with diversified structure design have been proposed to address this issue, it remains challenging to achieve a satisfactory TIM with both high through-plane thermal conductivity (κ_⊥) and low contact thermal resistance (R_contact) for meeting the practical application requirements. This study solves this problem by constructing a loosely packed and vertically aligned graphene monolith (VAGM), which was prepared by simply rolling up hybrid double-layer strips composed of porous polymer foam adhered onto the graphene paper, exhibiting an ultrahigh κ_⊥ of 276 W m^-1 K^-1. Moreover, a cap modification strategy by transferring the nanometer-thick gold (Au) foils onto both sides of VAGM was carried out to further optimize the contact state with roughness surface from heater/heat sink, finally giving a low R_contact of 0.41 K cm² W^-1 (double sides). As a result, our proposed graphene-based TIM exhibits an enhancement in cooling efficiency of ≈1.15 times compared to that of the state-of-the-art TIM (≈30 W m^-1 K^-1) in the TIM performance test, manifesting its superior ability to meet the ever-increasing heat dissipation requirement.

电子设备中的封装集成度和功率密度的迅速提高导致迫切需要高性能热界面材料（TIM），以有效解决伴随的热管理问题。尽管已提出了多种多样的高导热材料（例如石墨烯，碳纳米管和氮化硼纳米片）与多样化的结构设计相结合来解决此问题，但要获得令人满意的具有高贯穿面热导率（κ的TIM）仍然是一项挑战。_⊥）和低的接触热阻（ř_接触），以满足实际应用需求。本研究通过构建松散堆积和垂直排列的石墨烯整料（VAGM），它的制备是通过简单地卷起混合双层条带由粘附到所述石墨烯纸的多孔聚合物泡沫的，表现出超高解决了这个问题κ _⊥ 276 W的m ^-1  K ^-1。此外，通过将纳米厚的金（Au）箔转移到VAGM的两面，进行了瓶盖改性策略，以进一步优化与加热器/散热器的粗糙表面的接触状态，最终实现0.41 K cm的低R_接触² 瓦^-1（双面）。结果，与TIM性能测试中最先进的TIM（≈30 W m ^-1  K ^-1）相比，我们提出的基于石墨烯的TIM的冷却效率提高了约1.15倍，体现了其满足日益增长的散热要求的卓越能力。