Ce1−xZrxBiyO2−y/2 solid solutions were synthesized as new inorganic yellow pigments and their color properties have been investigated as possible ecological materials. Although the optical absorption edge of the Ce1−xZrxBiyO2−y/2 pigments depends on their composition, all samples absorb the ultraviolet and the visible light under 500 nm efficiently. As a result, the pigments show a brilliant yellow color, and the most effective yellow hue was obtained at x = 0.37 and y = 0.20. The importance of the presence of Bi3+ in the CeO2–ZrO2 lattice has been elucidated by comparing the color of Ce0.43Zr0.37Bi0.20O1.9 with that of Ce0.43Zr0.37La0.20O1.9. Characterization of the Ce1−xZrxBiyO2−y/2 solid solutions suggests that they have a potential to be alternative yellow colorants for paints, inks, plastics, and ceramics. Since they are composed of non-toxic and safe elements, they would be inert and safe and exhibit no side effects in the human body.