Li5La3Ta2O12:Mn4+ (LLTO:Mn4+) phosphors are prepared in air via high‐temperature solid‐state method and investigated for their crystal structures and luminescence properties. LLTO:Mn4+ phosphor under excitation at 314 nm shows deep‐red emission peaking at 714 nm due to the 2E→4A2 transition of Mn4+ ion. The excitation bands in the range 220 ‐ 570 nm are attributed to the Mn4+ ‐ O2‐ charge‐transfer band and the 4A2g→4T1g, 2T2g, and 4T2g transitions of Mn4+, respectively. The optimal Mn4+ ion concentration is ~0.4 mol%. The concentration quenching mechanism in LLTO:Mn4+ phosphor is electric dipole‐dipole interaction. The luminous mechanism and temperature quenching phenomenon are explained by the Tanabe‐Sugano energy level diagram and the configurational coordinate diagram of Mn4+ in the octahedron, respectively. The experimental results indicate that LLTO:Mn4+ phosphor has a potential application prospect as candidate of deep‐red component in light‐emitting diode (LED) lighting.

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