Low-cost and large-scale fabrication method of nanohole array, which comprises nanoscale voids separated by a few tens to a few hundreds of nanometers, has opened up new possibilities in biomolecular sensing as well as novel frontier optical devices. One of the key aspects of the nanohole array research is how to control the hole size following each specific needs of the hole structure. Here, we report the extensive study on the fine control of the hole size within the range of 500-2500 nm via surface-catalyzed chemical deposition. The initial hole structures were prepared via conventional photo-lithography, and the hole size was decreased to a designed value through the surface-catalyzed chemical reduction of the gold ion on the predefined hole surfaces, by simple dipping of the hole array device into the aqueous solution of gold chloride and hydroxylamine. The final hole size was controlled by adjusting reaction time, and the optimal experimental condition was obtained by doing a series of characterization experiments. The characterization of size-controlled hole array was systematically examined on the image results of optical microscopy, field emission scanning electron microscopy(FESEM), atomic-force microscopy(AFM), and total internal reflection microscopy.