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We report a newly developed surface engineering approach for TiO 2 nanoparticles toward transparent TiO 2 /silicone nanocomposites with high refractive index (RI) values. Zirconate coupling agents are adopted on the TiO 2 nanoparticles for surface passivation and to enhance the dispersibility of the nanoparticles in organic substrates. The modified TiO 2 nanoparticles can be uniformly dispersed in silicone, forming transparent hybrid films with an ultrahigh RI of 2.01. The preparation technique of colloidal TiO 2 and polymer-based nanocomposites is simple and suitable for scalable production, which is promising for expanding the application of TiO 2 materials in photonic devices.