The impact of attrition ball-mill pretreatment on food waste particle size, soluble chemical oxygen demand (SCOD), biochemical methane potential, and microbial community during anaerobic digestion was investigated based on milling speed and time. The uniformity of particle size improved with increasing milling speed and time. The SCOD of the pretreated samples increased to 4%, 7%, and 17% at the speeds of 150, 225, and 300 rpm, respectively, compared to the control. Milling time did not significantly change the SCOD. The cumulative methane productions of 430, 440, and 490 mL/g-VS were observed at the speeds of 150, 225, and 300 rpm, respectively, while the untreated sample exhibited the cumulative methane production of 390 mL/g-VS. Extended milling time did not improve methane production much. When the milling times of 10, 20, and 30 min were applied with the milling speed fixed at 300 rpm, the methane productions of 490, 510, and 500 mL/g-VS were observed respectively. Ball-mill pretreatment also increased the total volatile fatty acids. During the anaerobic digestion (AD) of ball-mill treated food waste, acetoclastic methanogens predominated, with a relative abundance of 48–49%. Interestingly, hydrogenotrophic methanogens were 1.6 times higher in the pretreated samples than those in the control. These results showed the potential of attrition ball milling as a food waste pretreatment for improving methane production.