Carbon capture materials play an important role in meeting global energy and climate goals. We conduct detailed computational investigations (DFT calculations, Monte Carlo simulation, etc.) of a wide spectrum of candidate materials, to achieve fundamental understanding of the chemical and structural interactions governing the carbon capture processes. Research topics include: sorption materials, carbon mineralization, catalytic conversion of CO2 into fuels, direct air capture, machine learning for large-scale material screening etc. Working closely with experimental teams at NIST, our computational efforts complement the experimental findings, help better understand the CO2 capture mechanisms, and suggest possible routes for improving existing materials and designing new materials.