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Lithium titanate with excess lithium (Li2+xTiO3+y) is one of the most promising candidates among advanced tritium breeders for demonstration power plant reactors because of its good tritium release characteristics. However, the tritium breeding ratio (TBR) of Li2+xTiO3+y is smaller than that of e.g., Li2O or Li8TiO6 because of its lower Li density. Therefore, new Li-containing ceramic composites with both high stability and high Li density have been developed. Thus, this study focused on the development of a solid solution with a new characteristic. The solid-solution pebbles of Li2+xTiO3+y with Li2ZrO3 (Li2+x(Ti,Zr)O3+y), designated as LTZO, were fabricated by an emulsion method. The X-ray diffraction patterns of sintered LTZO pebbles are approximately the same as those of Li2+xTiO3+y pebbles, and no peaks attributable to Li2ZrO3 are observed. These results demonstrate that LTZO pebbles are not a two-phase material but rather a solid solution. Furthermore, LTZO pebbles were easily sintered under air. Thus, the LTZO solid solution is a candidate breeder material for super advanced (SA) tritium breeders.