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This study presents the photoluminescence characteristic analysis of a series of red phosphors of KAlSiO4:1.5 mol%Sm3+,xmol%Eu3+(x = 2, 3, 4, 5, 6, 7) prepared via high-temperature solid-phase reaction. The results show that the X-ray diffraction (XRD) refinement results are reliable. The unit cell parameters and volume gradually decrease as the Eu3+concentration increases, resulting in a grain size reduction of 10.22%. When x = 6, the emission peaks of Sm3+at 564, 601, and 651 nm disappear completely, and the corresponding full width at half maximum becomes 0. At 610 nm, the emission peak intensity of Eu3+is increased by a factor of 4.8. The resonant non-radiative energy transfer effect is greater than the co-excitation effect. A maximum energy transfer efficiency of 97.8% is achieved. The integral area at 610 nm is as high as 85%. The color purity of the phosphor is as high as 92.97%, and the internal quantum yield gradually changes from 32% to 51%. Ultimately, these results confirm that the silicate phosphor is suitable for the red component in the three primary color phosphors of white light-emitting diodes.