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In the quest for eco-friendly optics, high refractive index polymers (HRIPs) with degradability have been one of the desirable optical materials for realizing eco-friendly and efficient lighting technologies. However, it has been challenging for HRIPs to simultaneously realize thermostability, high refractive index (RI), visible transparency, and efficient degradability, all of which are essential for their practical use. In this context, we herein focus on aromatic poly(dithioacetal)s, composed of visible-transparent yet degradable dithioacetal moieties and rigid phenylene sulfide spacers, exhibiting moderately high T g (> 60 °C), high RI (> 1.7), and colorless film features. In addition, poly(dithioacetal)s can balance (1) high stability under the operating conditions even upon heating and (2) quantitative degradability that can selectively yield cyclic low-molecular-weight products that can be further repolymerized upon further addition of an acid catalyst. These results provide a key concept for high refractive index polymers that allow on-demand degradability and recyclability without compromising their high potential thermal and optical properties., (© 2024 Wiley-VCH GmbH.)