A series of (Pr, Ce)-ZrSiO4 ceramic pigments were synthesized and characterized using XRD, SEM, EDS, XPS, XRF, colorimeter, and a UV-VIS-NIR spectrometer. The prepared pigments were mainly composed of the zircon phase and were well crystallized. Only a specific amount of Pr was incorporated into the ZrSiO4 lattice. Compared with Pr, Ce was almost completely incorporated into the ZrSiO4 lattice and was homogeneously distributed within the pigment particles. The dopant Ce reduced the amount of Pr dissolved in the ZrSiO4 lattice and thus caused the b* values of the samples to decrease slightly. Meanwhile, the presence of Ce induced an apparent increase in red tone in the samples. The enhanced red tone resulted primarily from an increase in the absorption of light with wavelengths between 500 and 565 nm. High-temperature stability analysis demonstrated that it is feasible to improve the tone of Pr-ZrSiO4 pigment by doping with Ce.