<p>This study explores the molecular design of sulfur-containing polymers with high refractive indices (RI) and optimized Abbe numbers for advanced optical applications. The high molar refraction and low dispersion of sulfur make it an ideal component for enhancing the optical properties of polymers. Density functional theory (DFT) calculations were employed to predict the RI and Abbe numbers for a range of sulfur-based polymers. To improve the accuracy of the theoretical predictions, a correction function was developed by comparing the calculated values with experimental data. The key polymer families investigated included sulfur-containing polycarbonates, heterocyclic optical resins, and cycloolefins, all modified to balance RI enhancement with dispersion control. The results demonstrate that increasing the sulfur content and introducing specific heterocycles and bridged rings can effectively increase the RI while maintaining desirable Abbe numbers. Polymers incorporating 1,4-dithiane and sulfur-bridged rings exhibit excellent optical clarity and minimal visible light absorption, making them suitable for lens and coating applications. The study also calculated the UV-visible spectra for the most promising polymers, confirming their high transparency. This work establishes a predictive framework for developing high-performance optical polymers and offers a systematic approach for balancing the refractive index and dispersion, thereby providing valuable insights for the design of next-generation optical materials.</p>