This study focused on the development of a solid solution with a new characteristic. Li2+xTiO3 powder was prepared by sol-gel method, and the pebbles was made by wet forming process. The X-ray diffraction patterns of sintered Li2+xTiO3 pebbles are approximately the same as those of Li2TiO3 pebbles, and no other peaks are observed. These results demonstrate that Li2+xTiO3 pebbles are not a two-phase material but rather a solid solution.