Tb4+-doped sodium zirconate samples, Na2Zr1−xTbxO3, were synthesized as novel environmentally friendly inorganic yellow pigments by a conventional solid-state reaction method. Their crystal structures, optical properties, and colors were characterized. A single-phase form was obtained for the samples in the x range of x ≤ 0.18, while impurity phases were detected for the sample with x = 0.20. All samples showed strong optical absorption in the blue light region, due to the charge transfer transition between O2− and Tb4+. As a result, the sample color became yellow, which is the complementary color of blue, and the color became more vivid with increasing Tb4+ content in the single-phase region. Among the samples, Na2Zr0.82Tb0.18O3 was the optimal composition, with the highest yellowness (b* = +67.2) and pure yellow hue (h° = 90.1). Although the b* value was lower than commercial yellow pigments such as BiVO4 and ZrSiO4:Pr, this sample had a purer yellow hue. Since Na2Zr0.82Tb0.18O3 is composed of non-toxic elements, it could be a new environmentally friendly inorganic yellow pigment.
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