Considerable amounts of anatase nanocrystals were formed on the (100 − x)SiO2·xTiO2 coatings with x of 16.5 and 25 mol% with boiling water treatment, whereas the formation of anatase nanocrystals was not clearly observed for the coatings with x of 50 and 75 mol%. Despite the lower TiO2 content, the coatings with x of 16.5 and 25 mol% showed higher concentration of Si–O–Ti bonds among the coatings. Thus, the hydrolysis of Si–O–Ti bonds and resultant sites should facilitate the nucleation and growth of anatase nanocrystals. High transparency, high photocatalytic activity, and superhydrophilicity were demonstrated for the anatase nanocrystals-precipitated coatings.