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Comprehensive Summary The merits of intrinsic electrical conductivity, high specific surface area, tunable chemical composition and tailor‐made properties enable two‐dimensional conductive metal‐organic frameworks (2D c‐MOFs) as promising next‐generation electrode materials in the field of energy storage and conversion. Herein, we have designed and synthesized a novel pyrazine‐based 2D c‐MOF (TPQG‐Cu‐MOF) bearing extended π‐conjugated structure and abundant redox active sites. Thanks to the excellent redox reversibility of pyrazine units and CuO 2 units, as well as the insolubility of the rigid framework skeleton, TPQG‐Cu‐MOF as the cathode material of lithium‐ion battery exhibits a reversible specific capacity (150.2 mAh·g –1 at 20 mAh·g –1 ), good cycling stability (capacity retention of 82.6% after 500 cycles at 1 A·g –1 ) and excellent rate performance. Comprehensive ex‐situ spectroscopic studies revealed the reversible redox activity of pyrazine units and CuO 2 units of TPQG‐Cu‐MOF during the Li + insertion/extraction process. The deepening fundamental understanding of the structure‐property relationship was proposed, which might pave the way for further development of efficient MOF‐based energy storage devices.
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