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A well-designed redox-active organic linker,pyrazine-2,3,5,6-tetracarboxylate（H4pztc）with brimming active sites for lithium ions storage was utilized to construct coordination polymers（CPs）via a facile hydrothermal reaction.Those two isostructural two-dimensional（2D）CPs,namely[M2（pztc）（H2O）6]n（M=Co for 1 and Ni for 2）,delivered excellent reversible capacities and stable cycling performance as anodes in lithium ion batteries.As demonstrated in electrochemical studies,1 and 2 can achieve highly reversible capacities of 815 and 536 mA h g-1at 200 mA g-1for 150 cycles,respectively,best performed for the reported2D-CP-based anode materials.The electrochemical mechanism studies showed that the remarkable performances can be ascribed to the synergistic Li-storage redox reactions of metal centers and organic moieties.Our work highlights the opportunities of using a well-designed organic ligand to construct low-dimensional CPs as new type of electrode materials for advanced lithium ion batteries.