The lithiated redox organic molecules containing the electrochemically active C=O functional group represent promising alternative electrode materials in portable electrochemical storage devices. Herein, terpyridine-based polycarboxylic acids (H3TPYTA = [2,2′:6′,2″-terpyridine]-4,4′,4″-tricarboxylate) were lithiated and used as starting materials to synthesize the novel lithium-rich iron supramolecular compound (LiFeTPYTA) and heterometallic-organic frameworks (CoFeTPYTA) with multi-redox active sites containing -[TPY-Fe(II)-TPY]- nodes (TPY = 2,2′:6′,2″-terpyridine). Upon application as anode material in Li-ion battery, LiFeTPYTA delivers a high specific capacity of 528 mAh g−1 at the current density of 100 mA g−1 after 100 cycles, while the capacity of CoFeTPYTA can be up to 1138.2 mAh g−1 at the current density of 100 mA g−1 after 300 cycles. Even at a current density of 5000 mA g−1, the electrode material maintains a capacity of 201.2 mAh g−1 after 5000 cycles. It is worth mentioning that such excellent cycle and rate performance outperforms most of the reported MOFs.