The red-emitting Sr 2 Si 5 N 8 :Eu 2+ phosphor with a superior quantum efficiency and suitable emission spectrum has been widely used as a promising down-conversion material in white light-emitting diodes. However, its thermal degradation under high temperature handicaps its large scale application, and therefore must be reduced. Here, we proposed to increase the thermal stability of Sr 2 Si 5 N 8 :Eu 2+ by coating a nanometer-order Al 2 O 3 film on each phosphor particle using an atomic layer deposition approach in a fluidized bed reactor. The deposited Al 2 O 3 layer was quite uniform and conformal when using O 3 as the oxidizer, and its thickness could be controlled by the dosage type, deposition temperature and cycle numbers, which largely affects the photoluminescence properties and thermal degradation of the title phosphor. Thermal gravimetric analysis results showed that the oxidation temperature of the coated phosphor increased from 700 to 850 °C, suggesting that the coating layer has the function of anti-oxidation. Meanwhile, the coated phosphor particle surface became hydrophobic. Consequently, the thermal degradation of phosphor powders in air at 200 °C was greatly reduced and the stability of the fabricated LEDs with coated powders was also improved. Prospectively, the proposed approach provides a new strategy to improve the thermal stability of other phosphors.