A Li (ion)–air cell was designed to investigate the reversible utilization of Li that was harvested from a cathode. In the Li (ion)–air cell, 0.1 M LiOH(aq) was used as the catholyte with oxygen in air and Li intercalation compounds such as graphite (C6) and Li4Ti5O12 (LTO) were used as the anodes. It appeared that the Li metal formed on the stainless-steel anode in the first charge of the Li–air cell was poorly reversible in further cycling owing to irreversible loss of Li during cycling. However, when Li intercalation compounds were used as anodes in a Li-ion–air cell, high coulombic efficiency by reversible reactions and good cycle performance were achieved. These results show that Li intercalation materials have significant potential as anode materials since they effectively utilize Li resources in Li–air battery systems and ensure reversibility in these systems.