A series of LiLaSiO4:yTm3+, zEu3+ phosphors were prepared by high temperature solid-phase reaction. The microstructure, luminescence performance and quantum yield of the phosphors are characterized by XRD, SEM and fluorescence spectrometer. When the monitoring wavelength is 360 nm, LiLaSiO4:yTm3+ phosphors showed a sharp emission peak at 460 nm, corresponding to the 7F0→5D2 energy level transition, and the concentration quenching point of Tm3+ ions was y = 0.015. When the monitoring wavelength is 360 nm, LiLaSiO4:yTm3+, zEu3+ phosphors have emission peaks of Tm3+ and Eu3+ ions at 460 and 618 nm, respectively. As the molar mass fraction of Eu3+ ions doped increases, the luminous intensity of Tm3+ ions gradually decrease, and the luminous intensity of Eu3+ ions increases first and then decreases, and the concentration quenching point of Eu3+ ions was z = 0.08. The energy transfer of Tm3+→Eu3+ ions through electric dipole- electric dipole interactions is demonstrated by the luminous intensity variation law and fluorescence lifetime. By changing the doping ratio of Eu3+ and Tb3+ ions, the full-color control of the phosphor luminescent color from blue to red can be achieved.