Wettability is one of the main parameters controlling CO2 injectivity and the movement of CO2 plume during geological CO2 sequestration. Despite significant research efforts, there is still a high uncertainty associated with the wettability of CO2/brine/rock systems and how they evolve with CO2 exposure. This study, therefore, aims to measure the contact angle of sandstone samples with varying clay content before and after laboratory core flooding at different reservoir pressures, of 10 MPa and 15 MPa, and a temperature of 323 K. The samples’ microstructural changes are also assessed to investigate any potential alteration in the samples’ structure due to carbonated water exposure. The results show that the advancing and receding contact angles increased with the increasing pressure for both the Berea and Bandera Gray samples. Moreover, the results indicate that Bandera Gray sandstone has a higher contact angle. The sandstones also turn slightly more hydrophobic after core flooding, indicating that the sandstones become more CO2-wet after CO2 injection. These results suggest that CO2 flooding leads to an increase in the CO2-wettability of sandstone, and thus an increase in vertical CO2 plume migration and solubility trapping, and a reduction in the residual trapping capacity, especially when extrapolated to more prolonged field-scale injection and exposure times.