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New phosphors with various emission colors for RE3+ doped Li1+xTa1−xTixO3 (LTT) (RE: Eu, Sm, Er, Tm, and Dy) were synthesized by electric furnace at 1423 K for 15 h. The microstructure of the host material and the photoluminescence (PL) property were determined and compared to those of RE3+ doped Li1+xNb1−xTixO3 (LNT). In the LTT phosphor, the highest PL intensity was achieved for the mixture composition Li1.11Ta0.89Ti0.11O3 with a LiTaO3 structure, although it has an M-phase superstructure. In the LTT host material, the effective activators were Eu3+ and Sm3+ ions, in contrast to the LNT host material. Here, we discuss the relationship between PL property and the host material’s structure.