Powder compacts of alkoxide‐derived fine silica powders were consolidated into a highly dense and uniform structure by ultra‐high‐pressure cold isostatic pressing of granules with controlled structure. The diameters of spherical and nearly monosized amorphous silica particles, prepared from metal alkoxide, were successfully controlled in the range of 9 to 760 nm by varying the concentration of ammonia. Close‐packed granules of these powders were produced by spray drying. These powders were isostatically pressed up to 1 GPa at room temperature. Although the average particle diameter was less than 100 nm, the maximum relative density of the compacts was more than 78% of theoretical density. The optimum particle size to obtain highly dense compacts was in the range of 30 to 300 nm at 1 GPa. Furthermore, the ratio of mode pore diameter in these compacts to particle diameter was less than 0.155, which corresponded to the minimum ratio of calculated three‐particle pore channel radii for hexagonal close packing. Viscous deformation of particles under ultra‐high isostatic pressure played an important role in the densification of t