A green submicro Cr‐ZrSiO4 pigment was successfully synthesized with Li2CO3 used as mineralizer by a simple solid‐state method at low temperature. The formations of the samples with and without mineralizer were investigated by X‐ray diffraction, scanning electron microscope, and thermogravimetry differential thermal analysis, respectively. The reflectance spectrum and color properties of the Cr‐ZrSiO4 pigments were characterized and analyzed. The XRD results show that Li2CO3 as a mineralizer can significantly promote the formation of ZrSiO4 and decrease the synthesis temperature to 900°C, which is 500°C lower than without mineralizer. The SEM revealed that the Li2CO3 containing ceramic powders are more homogeneous than undoped samples and have uniform particle size between 100 and 500 nm. It is indicated that Li2CO3 as a mineralizer can effectively destroy the Si‐O bond of random network structure, reduce the viscosity and accelerate the formation of ZrSiO4 at low temperature. The results from CIE L*a*b* characterization indicate that the samples exhibit high doping limitation (x = 0.06) and green hue (a* = −10.13) at 900°C. In addition, the method used in this work has the advantages of simple process, low cost, and large‐scale production, and is expected to synthesize other types of high‐temperature ceramic pigments.