The anti-reflection film can effectively reduce the surface reflectivity of solar photovoltaics, increase the transmittance of light, and improve the photoelectric conversion efficiency. The high refractive index coating is an important part of the anti-reflection film. However, the traditional metal oxide coating has poor stability and complicated processes. To address this issue, we prepared two organic high refractive index (HRI) photopolymers by modifying epoxy acrylic acid with 4,4′-thiodibenzenethiol, which can be surface patterned by nanoimprinting to prepare antireflection coatings. As a result, two modified photopolymers with high refractive index (n > 1.63), high optical transmittance (T > 95%), and thermal stability (Tg > 100 °C) are obtained after curing. In particular, the diphenyl sulfide photopolymer modified by ethyl isocyanate acrylate has a refractive index up to 1.667 cured by UV light. Our work confirms that the organic HRI photopolymer can be obtained by introducing high molar refractive index groups, with potential to be applied as a PV cell power conversion efficiency material.