Attempts were made to develop a stable gray pigment at reducing atmosphere, substituting Ti in $ZrTiO_4$ with Mn, Fe, Co and Cu The pigment synthesized at $1300~1500^{circ}C$ by solid state method with the composition of $ZrTi_{1-x-y}A_xB_yO_4$ (x = y = 0.005, 0.015, 0.035, 0.055, 0.075, 0.095, 0.115, 0.135, 0.155, 0.175 and 0.195 mole, A = Mn(III), Fe(III), Co(II, III) and Cu(II) (chromophores), B = Sb (counterion). The pigments were fired at $1400^{circ}C$ for 3 h with substitute amount changes of Mn, Fe, Co and Cu to $ZrTiO_4$ crystals, and analyzed by Raman spectroscopy to figure out substitute limits. Results indicated 0.035 mole for Mn, 0.115 mole for Fe, 0.015 mole for Co and 0.015 mole for Cu as substitute limits, respectively. Figs. 1, 2, 3, and 4 represent each substitute pigments of Mn, Fe, Co and Cu. Synthesized pigment was applied to a lime and a lime-magnesia glaze at 7 wt% each, and fired at reducing atmosphere of $1240^{circ}C$, soaking time 1h. Gray color was obtained with CIE-$L^*a^*b^*$ values at 44.55, -0.65, 1.19(Mn), 40.36, -0.90, 0.30(Fe), 42.63, -0.03, -1.49(Cu) and -40.79, -0.28, -0.91(Co), respectively.