This lecture will begin with an overview of energy-related capture, sequestration, conversion, and utilization of carbon dioxide (CO₂) [C.S. Song, Catal. Today, 115 (2006) 2–32; J. Am. Chem. Soc., 131 (2009) 5777-5783]. Carbon capture and sequestration (CCS) is considered as one of the key options for mitigating the emissions of CO₂ from energy systems. According to studies by US Department of Energy, CO₂ capture by current commercial technology using aqueous solutions of liquid alkanolamines is energy intensive and contributes to as much as two thirds of the total cost for CO₂ sequestration. We have proposed a new design concept of “molecular basket sorbent (MBS)” as a novel approach to CO₂ capture and separation using selective solid sorbent [X. Xu et al., Micropor. Mesopor. Materi., 62 (2003) 29-45].  CO₂ “molecular basket” is nano-porous, CO₂-selective high-capacity sorbent for adsorption separation of CO₂ from various gas mixtures. We have explored a number of new MBS formulations. An example of the MBS-CO₂ is a nano-porous composite of polyethyleneimine and a mesoporous moecular sieve MCM-41.  PEI-MCM41 type sorbents have been found to be effective for removing CO₂ from flue gas and other gas streams with high capacity and selectivity at 20-100 °C under atmospheric pressure. The CO₂ adsorption capacity and CO₂ separation selectivity of MCM-41 were greatly improved by loading PEI into its nano-sized pore channels (about 3 nm), which made the resulting sorbent operating like a “molecular basket” for CO₂ (MBS-CO₂).  The influence of moisture concentrations in the simulated flue gas on the CO2 adsorption separation performance was also examined. CO2 adsorption capacity of the MCM-41-PEI adsorbent for the simulated moist flue gas was higher than that for the simulated dry flue gas. The captured CO₂ can be easily and completely recovered by using a purge gas or a vacuum system at 75-100 °C.  The multi-cycle experiments have shown that the MBS-CO2 sorbents have very good regenerability and stability [C. S. Song et al., Stud. Surf, Sci. Catal., 153 (2004) 411-416].  With the MBS, CO₂ capture from flue gas can be conducted in a solvent-free and compact solid sorbent system more energy efficiently, economically and environmentally friendly. The MBS-CO₂ concept has also been found applicable to capture and separation of hydrogen sulfide H₂S in gas mixtures [X. Wang et al., Green Chemistry, 9 (2007) 695-702; J. Phys Chem C, 113 (2009) 7260-7268].   Results of analytical characterization of MBS will also be discussed to shed light on why and how these novel sorbents work under realistic conditions.