The problem of thermal management of electronic devices leads to high demand of thermal interface materials (TIMs) with high thermal conductivity (TC) and softness. In this work, graphite foam (GFoam) was used to fabricate silicon rubber (SR) matrix-based TIMs by stacking and vertical cutting method. The obtained 75 vol% GFoam(100)/SR shows a high through-plane TC of 330.33 W m−1 K−1 due to the vertically aligned graphite layers. A strong correlation between the properties of the composites and the density of the fillers is found, providing a new perspective to adjust the properties of the composites. Composites with different proportions of GFoam and graphite film (GF) were prepared to further enhance the mechanical properties without obvious sacrifice of the thermal management performance. We believe that the design principles proposed in this work will be important for developing high-performance thermal management materials.
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