A zirconia/oligosiloxane nanocomposite encapsulant has been developed and tested in a high-power LED package against commercial silicone resins. The composite was a marriage of zirconia nanocrystals modified with butyric acid (BA) and 3-methacryloxy propyl trimethoxysilane (MPTMS) and a high-index methacryloxy-oligosiloxanes resin made from MPTMS plus dimethyl, diphenyl, and triphenyl silanes. The modified zirconia had an index of 1.762 (@589 nm) and was dispersible in many solvents. The oligosiloxane resin, however, had an index of 1.5413 with good encapsulation properties and low viscosity allowing the incorporation of more zirconia. The final nanocomposite showed a refractive index of 1.625 with high transparency and a wavelength-independent scattering, both desirable for the light extraction from LED. When tested in a high-power LED package, the composite encapsulant resulted in 13% more light output compared to the commercial encapsulant (OE-6630, Dow Corning Corp.) and showed longer than 1000 h of lifetime (L70) under the steady-state Temperature Humidity Bias (THB) test. (Graph Presented).