Using a convenient solid-state reaction Ce 0.67 Tb 0.33 Mg 1-x Mn x Al 11 O 19 green phosphors were prepared. The effect of Mn 2+ + doping on the luminescence properties, energy transfer mechanism, and color gamut under 254 nm excitation were investigated. The energy transfer from (Ce,Tb) 3+ + to Mn 2+ + was found to be due to multipolar interactions of the dipolequadrupole mechanism from theoretical fitting results. The critical distance was calculated to be 0.797 nm. When the Mn 2+ + doping content was increased from 0 to 0.12, the energy transfer efficiency (Ce 3+ + ,Tb 3+ + ? Mn 2+ + ) gradually increased from 0% to 58%. The Ce 0.67 Tb 0.33 Mg 0.88 Mn 0.12 Al 11 O 19 sample exhibits 105% of the standard NTSC color gamut. Results indicate that Ce 0.67 Tb 0.33 Mg 0.88 Mn 0.12 Al 11 O 19 green phosphors can be applied to illumination devices and displays.