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The development of polymeric optical materials with a higher refractive index, transparency in the visible spectrum region and easier processability is increasingly desirable for advanced optical applications such as microlenses, image sensors, and organic light-emitting diodes. Most acrylates have a low refractive index (around 1.50) which does not meet the high performance requirements of advanced optical materials. In this research, three novel acrylates were synthesized via a facile one-step approach and used to fabricate optical transparent polymers. All of the polymers reveal good optical properties including high transparency (≥90%) in the visible spectrum region and high refractive index values (1.6363) at 550 nm. Moreover, nanostructures of these acrylate polymers with various feature sizes including nanogratings and photonic crystals were successfully fabricated using nanoimprint lithography. These results indicate that these acrylates can be used in a wide range of optical and optoelectronic devices where nanopatted films with high refractive index and transparency are required.