Caprock sealing capacity is paramount for the safety and efficacy of geological carbon storage. This study investigates the evolution of mudstone caprock sealing capacity under CO₂–mechanical coupling, integrating experimental rock mechanics with fluid–solid coupling numerical simulations. Laboratory experiments reveal that caprock permeability exhibits strong stress sensitivity, decreasing exponentially with increasing effective stress. The stress sensitivity coefficient is highly dependent on initial pore pressure and porosity, being greatest under low-pore-pressure and high-porosity conditions. Furthermore, permeability loss during loading is partially irreversible due to plastic deformation. Numerical simulations, conducted using an integrated Petrel + Visage + Eclipse workflow, quantify the influence of caprock physical and mechanical properties on sealing capacity during CO₂ injection. The results demonstrate that vertical total stress increases with increasing porosity, Young’s modulus, and permeability, with permeability exerting the most significant control. Conversely, vertical effective stress decreases with increases in these parameters, with porosity causing the largest variation. We conclude that lower caprock permeability and porosity are most critical for enhancing sealing integrity, while a higher Young’s modulus improves mechanical stability. These findings provide a theoretical basis and practical methodology for evaluating caprock sealing capacity and ensuring the secure storage of CO₂.