The purpose of this study was to determine the optimal firing condition and composition for $Al_2TiO_5$ crystal, which is suitable for stable coloration in glazes at high temperatures, using $Cr_2O_3$ as chromophore for the synthesis of $Al_2TiO_5$ system pigments. $Al_2TiO_5$ has a high refractive index and good solubility of chromophore in the $Al_2TiO_5$ lattice, making this structure a good candidate for the development of new ceramic pigments. Pigments were synthesized by using $Al_2O_3$ and $TiO_2$ mainly. Various amounts of $Cr_2O_3$ such as 0.01, 0.02, 0.03, 0.04 and 0.05 mole were also added. Each compound was synthesized at $1300^{circ}C$, $1400^{circ}C$, and $1500^{circ}C$ for 2 hours and cooled naturally. The crystal structure, solubility limit, and color of the synthesized pigments were analyzed by XRD, SEM, Raman spectroscopy, UV and UV-vis. The changes in color as the result of applying 6 wt% of the synthesized pigments to lime barium glaze were expressed as CIE-L*a*b* values. A $Cr_2O_3$ 0.03 mole doped $Al_2TiO_5$ brown pigment was successfully synthesize at $1400^{circ}C$, and the values of CIE-L*a*b* parameters were L* = 44.62, a* = 3.10, and b* = 17.25. In the case of the pigment synthesized at $1500^{circ}C$, the brown color was obtained at 0.01 mole and 0.02 mole $Cr_2O_3$, and the CIE-L*a*b* values were 55.34, 1.73, 28.64, and 49.39, 0.51, 21.33, respectively. At $1500^{circ}C$, the maximum limit of solid solution was 0.03 mole $Cr_2O_3$. The glazed sample showed green color, and the values of the CIEL* a*b* parameters were L* = 45.69, a* = -0.98, and b* = 20.38.