A lithium-oxygen battery would deliver the highest energy density of a rechargeable battery, but the multiphase electrochemical reaction on the air cathode has difficulty proceeding when operated with only solid catalysts. We report here the organic-electrolyte-dissolved iron phthalocyanine (FePc) as a shuttle of (O2)(-) species and electrons between the surface of the electronic conductor and the insulator Li2O2 product of discharge. The Li2O2 is observed to grow and decompose without direct contact with carbon, which greatly enhances the electrochemical performance. Our results signal that the use of molecular shuttles that are catalytically active may prove to be enablers of a practical lithium-air rechargeable battery.