The establishment of a sustainable CO2 cycle displays a high-priority target of global climate protection, and energy effciency and environmental care in particular. The envisaged project aims at a molecular understanding of reversible CO2 uptake from air and subsequent catalytic transformation of CO2 to sustainable compounds/materials. Such implementation of an energy and resource-effective CO2 cycle is an ambitious goal. Our approach is based on the recently discovered chemistry of rare-earth-metal coordination compounds with carbon dioxide. The innovative concept takes advantage of the special reactivity of naturally occuring nitrogen compounds toward CO2. Synergistic effects of metal complexes and porous materials can be anticipated. The working hypothesis is applied to nontoxic light metals with similar properties (and reactivities) as found for the rare-earth metals, ideally minimizing any “energy penalty” as well as “mass penalty”.