Flake graphite has excellent explosive electron emission performance for its plenty surface micro-bulges and high graphitization degree, but its advantages have rarely been studied in relativistic magnetrons. In this paper, flake graphite cathodes with different fineness were used in coaxial diodes and relativistic magnetrons, and the influence of the surface microstructure of the flake graphite cathode on the relativistic magnetron performance is demonstrated for the first time. The result showed that the graphite microstructure mainly affected the initiation stage of explosive emission. Moreover, the delay time is determined by the degree of graphitization and the surface microstructure of graphite, and the surface microstructure plays a major role. Under the applied voltage of ∼ 330kV-∼ 490kV, The finer flake graphite possessed a shorter emission delay and facilitated the microwave excitation. The excitation time of finer flake graphite is ∼ 3ns, and ∼ 5ns for lager flake graphite. After several operations of the relativistic magnetron, the edges of flake graphite were blunted, and the surface of the flake graphite appeared droplet-like areas formed by anode atom sputtering. This work reveals the advantages of the finer flake graphite cathode in the fast priming of the relativistic magnetron, thus shedding new light on cathode design of the relativistic magnetron.