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The mechanical properties especially the compression performance are very important for thermal interface materials (TIMs) to mitigate warpage failure caused by stress concentration and reduce contact resistance in practical applications. However, high thermal conductivity and excellent mechanical properties are generally incompatible in traditional TIMs. Herein, we fabricate a high-performance carbon fiber-based TIM by using an extrusion method based on the flow shearing effect. The vertically oriented composite shows a through-plane thermal conductivity up to 18.5 W·m−1·K−1 at 20 wt% carbon fiber content, which is 92.7 times that of pure matrix and 6.3 times that of the random structure. Moreover, the as-prepared material exhibits low hardness of 56 (Shore 00) and outstanding elastic compression performance of 51.4% compression under a pressure of 45 psi. These excellent properties are primarily attributed to the high orientation of the carbon fibers (CFs), thereby establishing a direct and effective thermal conductivity path in the vertical direction. In addition, the synergistic effect of carbon fibers and alumina particles is also beneficial for building thermal conduction pathways. Our work provides an insight to further research in fabricating high-performance flexible TIMs as a promising candidate for applying in advanced thermal management fields. • The composite achieves a thermal conductivity of 18.54 W·m−1·K−1. • The composites exhibit good elastic compliance under high through-plane thermal conductivity. • The synergistic effect of carbon fibers and alumina promotes the enhancement of thermal conductivity [ABSTRACT FROM AUTHOR]