In a process for separating impurities from a raw gallium material containing impurities, a process for refining gallium comprising progressively solidifying a raw gallium material provided in a liquid state inside a vessel while applying stirring, such that the diameter of the tubular solidification boundary gradually advances from the inner wall plane of the vessel towards the center of the vessel to reduce the diameter of the tubular solidification boundary, and separating the liquid phase remaining in the central portion of the vessel from the solidified phase before the entire raw material inside the vessel is solidified. The process above is repeated as required by using, as the raw gallium material, the solidified phase from which the liquid phase is separated. A metallic gallium favorably used for the preparation of a compound semiconductor can be obtained by analyzing the impurity concentration of the impurity-concentrated Ga separated from the solidified layer.