In a very recent article (Chem.-Eur. J. 2014, 20, 6636), Olson et al. performed a theoretical study of the low-lying isomers of Li3N3 and found that two of the most stable structures show a novel N-3(3-) molecular motif, which possesses structural and chemical bonding features similar to ozone. We explore a first application of these new Li3N3 species as a captor of carbon dioxide. Our results conclude that this is a very exothermic and exoergic process (the capture of one and two carbon dioxide molecules on Li3N3 releases, respectively, 42 and 70 kcal mol(-1) in relative free energy values evaluated at the CCSD(T)/aug-cc-pVTZ//B3LYP/aug-cc-pVTZ level of theory), which apparently occurs without any energy barrier but requires a nonlinear N-3(3-) molecular motif.