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This study focused on the importance of the interfacial adhesion in the zirconia (ZrO₂)/silicone hybrids as the encapsulating material on the reliability of the LEDs. Surface-modified ZrO₂ nanoparticles (m-ZrO₂) with functional groups were prepared by a sol-gel reaction which could become reactive to the silicone resin. The produced m-ZrO₂/silicone hybrid at 5 wt% had a refractive index of 1.569 at 633 nm and light transmittance of 98.9%. Moreover, the coefficient of thermal expansion was greatly reduced by the introduction of m-ZrO₂ into the silicone resin. When using this m-ZrO₂/silicone hybrid, the luminous flux of the LED was 10.1% higher than that using a neat silicone resin. Most importantly, the LEDs encapsulated with the m-ZrO₂/silicone had the best performance under thermal shock among all the LEDs tested in this study, owing to its strong interfacial adhesion between the nanoparticles and matrix …