Climate change due to anthropogenic carbon emissions is a global issue and its mitigation requires scientific advancements in the areas of carbon dioxide capture, conversion, and storage. Capture of industrial point-source carbon dioxide emissions and subsequent sequestration by means of injection into the pore space of geological formations may provide long-term storage opportunity. However, our knowledge of the physical and chemical processes that determine the efficiency of carbon dioxide capture and storage, respectively, is limited. Accelerating scientific discovery and improving our understanding of the critical molecular-scale phenomena is needed. In the first part of this presentation, I will introduce our team’s research approach to materials discovery in carbon capture. In the second part, I will present our research progress in the area of carbon dioxide injection, trapping and storage at pore scale. To that end, we have developed a “digital rock” simulation environment in which we create high-accuracy capillary network representations  for numerical and statistical analyses of the connected pore space in geological samples. Within the capillary networks, we simulate the flow of complex fluids, including carbon dioxide and brine, at realistic reservoir conditions. Specifically, we have performed series of flow simulations at elevated pressures and temperatures in which brine is displacing super-critical carbon dioxide and vice versa, for quantifying the saturation levels in capillary networks of reservoir rock. We are currently extending our computational research to include an experimental, rock-on-chip microfluidics approach for validating the flow simulation results. Going forward, the inclusion of carbon dioxide related dissolution and mineralization dynamics at pore scale is necessary for unlocking the potential of geological carbon storage at large scale.