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 the compacts.