Zirconium silicate (ZrSiO4) powders with different doping concentrations of Mn4+ were prepared by solid-state reactions. The effect on the photoluminescence properties of ZrSiO4∶Mn4+ was studied. The structure of ZrSiO4∶Mn4+ was analyzed by X-ray powder diffractometer (XRD). The result shows that the powder was completely synthesized at 1 400 ℃. The spectral properties of ZrSiO4∶Mn4+ powders at different doping concentrations were studied. The best luminescence performance was obtained at 0.3%Mn4+ doping concentration. In the excitation spectrum, the peak at 363 nm is caused by the superposition of the charge transfer band of O2--Mn4+ and the 4A2-4T1 energy level transition of the spin-allowed Mn4+, while the peak at 450 nm is caused by the 4A2-4T2 energy level transition of the Mn4+. The main emission peaking at 667 nm was due to the spin-forbidden transitions 2E-4A2 of Mn4+. The other peak located at 698 nm was caused by anti-stokes vibronic sidebands associated with the excited state 2E of Mn4+. The decay curves show that the lifetime of ZrSiO4∶0.1% Mn4+ powders is 0.204 1 ms. The results show that ZrSiO4∶Mn4+ powders have good luminescent properties, they have the potential to be used in LED lighting industry.