Granulation is an ancient and sophisticated decorative technique. The production of granules is a crucial part of this process but has rarely been studied. The present study employed three techniques—pouring method, heating method, and crucible method—to produce gold granules. The success ratio of granule formation, granule surface morphology, microstructure, and formation were analyzed to identify the techniques used in archaeological objects. The cooling medium significantly influenced small granule formation, microstructure, and grain size. Both heating and crucible methods could control the granule formation, but these methods produced distinct microstructures. Based on these experimental granules, the probable production methods of ancient gold balls were identified. The present study provided microscopic information for determining ancient gold granule production techniques.