Activated carbon (AC) with a very high specific surface area of >3000 m2 g−1 and a number of course particles (average size: 75 µm) was pulverized by means of planetary ball milling under different conditions to find its greatest performances as the active material of an electric double-layer capacitor (EDLC) using a nonaqueous electrolyte. The variations in textural properties and particle morphology of the AC during the ball milling were investigated. The electrochemical performance (specific capacitance, rate and cyclic stabilities, and Ragone plot, both from gravimetric and volumetric viewpoints) was also evaluated for the ACs milled with different particle size distributions. A trade-off relation between the pulverization and the porosity maintenance of the AC was observed within the limited milling time. However, prolonged milling led to a degeneration of pores within the AC and a saturation of pulverization degree. The appropriate milling time provided the AC a high volumetric specific capacitance, as well as the greatest maintenance of both the gravimetric and volumetric specific capacitance. A high volumetric energy density of 6.6 Wh L−1 was attained at the high-power density of 1 kW L−1, which was a 35% increment compared with the nonmilled AC. The electrode densification (decreased interparticle gap) and the enhanced ion-transportation within the AC pores, which were attributed to the pulverization, were responsible for those excellent performances. It was also shown that excessive milling could degrade the EDLC performances because of the lowered micro- and meso-porosity and the excessive electrode densification to restrict the ion-transportation within the pores.