Deformable surface design of vertical graphene thermal interface materials for efficient heat dissipation

Vertical graphene, serving as a thermal interface material (TIM), is very promising for efficient thermal dissipating. Yet, the heat-dissipating efficiency is mediocre since satisfactory through-plane thermal conductivity ( κ ⊥ ) and contact thermal resistance ( R contact ) cannot be obtained simultaneously. In this work, we achieve TIMs with ultrahigh κ ⊥ (738.6 W m −1 K −1 ) and low R contact (29.2 K mm 2 W −1 ) based on volume shrinkage of silver paste within vertical graphene monoliths (VGMs). The outstanding κ ⊥ derives from vertically arranged graphene films (GFs) with excellent in-plane thermal conductivity. Besides, the silver pastes between GFs shrink after heating, triggering exposure of soft GF ends and forming a deformable surface to realize a notable decrease in R contact . Our VGM TIMs display an enhancement in thermal dissipating efficiency of ∼2.44 times compared to that of the state-of-the-art TIMs. Our findings offer practical design guidelines for advanced TIMs and thermal management applications.