Graphite is the most commonly used large-area cathode material in the high-power vacuum electron device for its long life and good repetitive-frequency performance, but its particle size selection scheme has not been elucidated. Therefore, in the present work, the explosive electron emission properties of flake graphite large area explosive electron emission cathodes with varied particle sizes are studied. The 320 mesh flake graphite has a current delay reduction of 0.2–0.9 ns compared to other samples at the same peak voltage. According to the Murphy–Good equation, the emission performance of each sample during the priming stage was calculated, and the threshold characteristics of 320 mesh flake graphite were significantly better than the other samples. After the space charge limited current is formed, the plasma expansion rate of all samples is 1.2±0.2cm/μs with a difference not exceeding 4% between samples. Our research provides a strong basis for the selection of raw materials for graphite based large area explosive electron emission cathodes and contributes to the development of cross-field high-power vacuum devices.