Vacuum hot‐press sintering process is utilized to manufacture graphite flake/aluminum composites, and the influence of graphite flake volume fraction on the microscopic structure, hardness, thermal conductivity (TC) and coefficient of thermal expansion (CTE) of the composites are investigated. The results indicate that the graphite flakes are neatly aligned along the in‐plane direction in the composites and exhibit a strong bond with the aluminum matrix interface. The in‐plane TC of the composite significantly increase with the addition of graphite flakes, whereas hardness, through‐plane TC, and the CTE decrease. As the volume fraction of graphite flakes in the composites increase from 15% to 60%, in‐plane TC improve from 278.8 to 353.8 W m–1 K–1, through‐plane TC decrease from 164.4 to 33.2 W m–1 K–1, and the CTE decrease to 13.7 × 10–6 K–1, achieving high thermal conductivity and a low coefficient of thermal expansion.This article is protected by copyright. All rights reserved.