Petroleum pitch‐based graphite blocks (GBs) attract considerable attention owing to their low cost, high yield, and possible application as heat sink components. However, no studies have systematically investigated the particle size distribution of GBs, their structures, and the relationship between the structures and thermal properties resulting from graphitization. Hence, herein, we present a novel method for fabricating petroleum pitch‐based GBs using natural graphite flakes (GFs) of sizes ranging between 50 and 500 μm and a bimodal particle size distribution. Furthermore, the effects of the mean GF particle size, pitch binder content, and microstructure of the GBs with low GF contents on compression molding with elevated hot‐pressing temperatures after graphitization are investigated. To investigate the effect of packing density with a GF size of 500 μm, we mix a small‐sized GF (50 μm) and low pitch binder content by kneading. In particular, specimens in the in‐plane direction with a bimodal particle size distribution of GFs and 10 wt% pitch binder yield optimum density and thermal conductivity values of 1.74 g m−3 and 384 Wm−1 K−1, respectively, after high‐temperature graphitization at 2600°C. These findings provide insights for developing high‐performance GBs for use in heat sink components with high thermal conductivity.
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