CO2 capture, storage and utilization (CSU) have become worldwide concerns due to an increasing awareness of the link between CO2 accumulation in the atmosphere and global warming. Layered double hydroxide (LDH)-derived compounds (LDOs) are recognized as important intermediate-temperature (200–400 °C) CO2 adsorbents for pre-combustion CO2 capture, particularly for the sorption enhanced water gas shift (SEWGS) and sorption enhanced steam reforming (SESR) processes. LDOs have been investigated for decades as CO2 adsorbents and great efforts have been devoted to improving their CO2 capture capacities and long-term stability. In this chapter, the research progress on the performance of LDH-derived CO2 adsorbents will be critically reviewed, including influence of the chemical composition of LDHs, synthetic conditions and methods, LDH-based composites, doping with alkali metals, other co-existing gases, the adsorption mechanism and kinetics, and techno-economic assessment. In addition, new research directions for further study will be proposed. We hope this critical chapter will not only summarize the main research activities in this area, but also shed light on future developments and possible links between fundamental studies and industrial applications, as well as give suggestions for future research efforts.