In this study a holistic approach to studying novel materials for carbon capture and storage is presented, encompassing the entire design of new materials from theoretical screening to experimental validation and in situ studies to probe their performance in real time. In the fi rst part, a high throughput screening methodology was devised to function within the Materials Project database. The screening found 640 materials that could be potentially implemented in high temperature carbonate looping; the materials were subsequently ranked by the theoretical energy penalty associated with their use. The most promising candidates were synthesised and subjected to thermogravimetric and diffraction studies to determine their experimental carbonation behaviour, showing good agreement with the screening results. The second part describes a study of the rst perovskite-type material shown to reversibly react with CO2, Ba4Sb2O9. A combination of in situ thermogravimetric, diffraction and imaging techniques were used to characterise the structural evolution of the material and its stability upon repeated carbonation cycles. Remarkably stable capacity retention over 100 cycles was found, a key improvement over currently used materials. The final part details the use of novel solid-state nuclear magnetic resonance techniques to study how ion dynamics influence the CO2 absorption properties of alkali oxides. Using measurements collected up to the high operating temperatures of these CO2 capture materials, it was found at higher temperatures the Li and O ionic dynamic processes are correlated, and the range of increased mobility coincides with the range over which CO2 absorption takes place. These results present initial insights into the underlying mechanism of CO2 capture in these materials, and how ion dynamics in influence their absorption kinetics.