Considerable attention has been paid to metal-organic frameworks (MOFs) for applications as electrode materials for lithium-ion batteries recently. In this study, we use cobalt terephthalate CoC8H4O4 (CoTPA), one type of MOFs, as an anode material for lithium-ion batteries for the first time. It delivers a high discharge capacity of about 700 mAh g−1 after 100 cycles with superior capacity retention. In contrast to the conventional lithium-storage mechanism of MOF-based anodes in organic carbonyl units, both the inorganic unit (Co2+) and the organic unit (carbonyl group) offer multi-electron transfer reactions, which results in such a high capacity.