Highly ordered mesoporous silica particles with sizes in the micron to sub-micron range are of great interest due to their applications as catalysts and filler materials. Currently, mesoporous silica particles are synthesized using large amounts of solvent, which is impractical for large scale-up in industry. This paper reports on a high-energy ball milling process that has been employed to create micron to sub-micron sized mesoporous silica particles starting from a silica xerogel prepared by a surfactant self-assembly sol-gel process. We have studied the effect of parameters such as milling media (e.g., zirconia, stainless steel, and steel centered nylon balls), milling time, the presence of surfactants during milling, particle size, and pore structure. Results from transmission electron microscopy (TEM), scanning electron microscopy (SEM), Xray diffraction (XRD), and nitrogen adsorption demonstrate the feasibility of producing large quantities of mesostructured particles by a simple milling process.