Herein, we explore the intrinsic ability of cellulose dissolved in NaOH(aq) to reversibly capture CO 2 . The stability of cellulose solutions differed significantly when adding CO 2 prior to or after the dissolution of cellulose. ATR-IR spectroscopy on cellulose regenerated from the solutions, using ethanol, revealed the formation of a new carbonate species likely to be cellulose carbonate. To elucidate the interaction of cellulose with CO 2 at the molecular level, a 13 C NMR spectrum was recorded on methyl α-D-glucopyranoside (MeO-Glcp), a model compound, dissolved in NaOH(aq), which showed a difference in chemical shift when CO 2 was added prior to or after the dissolution of MeO-Glcp, without a change in pH. The uptake of CO 2 was found to be more than twice as high when CO 2 was added to a solution after the dissolution of MeO-Glcp. Altogether, a mechanism for the observed CO 2 capture is proposed, involving the for-