Holographic data storage, due to its potential to increase capacity beyond one terabyte per disk, is tipped to be one of the next generation optical data storage technologies. Polymer-based systems are leading candidates due to their high dynamic range, high sensitivities, and flexible and easy production, and yet polymerization-shrinkage-induced distortion is a major hurdle for its reliable use. In this paper, a new free radical polymerization holographic recording medium, based on low shrink cyclic allylic sulfides (LS-CASs) ring-opening monomers, is proposed and demonstrated. The percentage of volume shrinkage is measured to be 0.02%, with refractive index (RI) contrast of (1.01 ± 0.5) × 10−3. The measured volume shrinkage is, to the authors' best knowledge, the best reported so far in the literature. Other parameters such as sensitivity, dynamic range, and dark reaction properties are also measured, where the values can be optimized with high RI functional groups without sacrificing the low shrinkage.