Abstract: Carbonated decomposition of hydrogarnet is one of the vital reactions of the calcification–carbonation method, which is designed to dispose of low-grade bauxite and Bayer red mud and is a novel eco-friendly method. In this study, the effect of the silica saturation coefficient (x) on the carbonation of hydrogarnet was investigated from the kinetic perspective. The results indicated that the carbonation of hydrogarnets with different x values (x = 0.27, 0.36, 0.70, and 0.73) underwent two stages with significantly different rates, and the kinetic mechanisms of the two stages can be described by the kinetic functions R3 and D3. The apparent activation energies at Stages 1 and 2 were 41.96–81.64 and 14.80–34.84 kJ/mol, respectively. Moreover, the corresponding limiting steps of the two stages were interfacial chemical reaction and diffusion.