Optical materials with high refractive index (n) have been rapidly improved because of urgent demands imposed by the development of advanced photonic and electronic devices such as solar cells, light emitting diodes (LED and Organic LED), optical lenses and filters, anti-reflection films, and optical adhesives. One successful method to obtain high refractive index materials is the blending of metal oxide nanoparticles such as TiO2 and ZrO2 with high n values of 2.1–2.7 into conventional polymers. However, these nanoparticles have a tendency to agglomerate by themselves in a conventional polymer matrix, due to the strong attractive forces between them. Therefore, there is a limitation in the blending amount of inorganic nanoparticles. In this paper, various hydrophilic polymers such as poly(N-hydroxyl acrylamide) (pHEAAm), poly(vinyl alcohol), poly(ethylene glycol), and poly(acrylic acid) were examined for preparation of high refractive index film based on titanium oxide nanoparticle (TiNP) dispersed polymer composite. The hydrogen bonding sites in these hydrophilic polymers would improve the dispersibility of inorganic nanoparticles in the polymer matrix. As a result, pHEAAm exhibited higher compatibility with titanium oxide nanoparticles (TiNPs) than other water-soluble polymers. Transparent hybrid films were prepared by mixing pHEAAm with TiNPs and drop casting the mixture onto a glass plate. The refractive indices of the films were in good agreement with calculated values. The compatibility of TiNPs with pHEAAm was dependent on the surface characteristics of TiNPs. TiNPs with the highest observed compatibility could be hybridized with pHEAAm at concentrations of up to 90 wt%, and the refractive index of the corresponding film reached 1.90. The high compatibility of TiNPs with pHEAAm may be related to the hydrophilicity and amide and hydroxyl moieties of pHEAAm, which cause hydrogen bond formation on the TiO2 surface. The obtained thin film was slightly yellow due to the color of the original TiNP dispersion; however, the transmittance of the film was higher than 80% in the wavelength range from 480 to 900 nm.