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Mn⁴⁺-doped red-light-emitting phosphors have become a research hotspot that can effectively enhance photosynthesis and promote morphogenesis in plants. Herein, the red phosphor La₃Mg₂NbO₉:Mn⁴⁺ was synthesized through the solid-state reaction method. The effects of adding H₃BO₃ and a charge compensator R⁺ (R = Li, Na, K) on the crystal structure, morphology, quantum efficiency, and luminous performance of the La₃Mg₂NbO₉:Mn⁴⁺ phosphor were systematically analyzed, respectively. The results showed that adding H₃BO₃ flux and a charge compensator improved the quantum efficiency and luminescence intensity. The emission intensity of the phosphor was enhanced about 5.9 times when Li⁺ was used as the charge compensator, while it was enhanced about 240% with the addition of H₃BO₃ flux. Remarkably, it was also found that the addition of H₃BO₃ flux and a charge compensator simultaneously improved the thermal stability at 423 K from 47.3% to 68.9%. The prototype red LED fabricated using the La₃Mg₂NbO₉:Mn⁴⁺,H₃BO₃,Li⁺ phosphor exhibited a perfect overlap with the phytochrome absorption band for plant growth. All of these results indicate that the La₃Mg₂NbO₉:Mn⁴⁺,H₃BO₃,Li⁺ phosphor has great potential for use in agricultural plant lighting.