During the first decades of geologic CO2 storage in saline formations and depleted reservoirs, structural trapping is the most important storage mechanism. The effectiveness of CO2 containment hinges on the assumption that the sealing formation remains water wet in the presence of dense CO2. In this work, multiple 13C and 1H magnetic resonance (MR) methodologies were employed for the first time to evaluate the interactions between supercritical CO2, brine, and the pore surface of a Berea sandstone core plug under reservoir conditions. These studies employed a novel variable field superconducting MR and magnetic resonance imaging (MRI) instrument which permitted sequential 1H and 13C measurements of core plugs at high-pressure and high-temperature. To systematically study the wettability of rock core exposed to supercritical CO2, four experiments were designed including bulk CO2 in a high-pressure vessel, bulk CO2-brine, 13CO2 in dried rock core, and a 13CO2-brine-rock experiment.The measured 13C and 1H MR relaxation times in this work indicate that the Berea sandstone remained strongly water-wet when the brine saturated core plug was exposed to supercritical CO2 under reservoir conditions. For both 13C and 1H, T1 relaxation times provide more reliable wettability evaluation as compared to T2 due to the impact of molecular diffusion through internal magnetic field gradients. One-dimensional (1D) MRI was employed to spatially resolve 13CO2 and brine in the core plug. Two-dimensional (2D) MRI was able to image 13CO2 and brine in a PEEK vessel. The quantities of CO2 and brine in the core plug were determined from the MR signal intensities of 13CO2 and brine.