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The manufacturing process for electrodes in lithium-ion batteries generally results in a nonuniform microstructure geometrically distributed in the through-thickness direction of an electrode. A porous structure was designed to decrease tortuosity and increase Li+ penetration in a thick Li4Ti5O12 (LTO) electrode. By using NaCl as a template, the porous LTO electrode with a high mass loading of 12 mg cm–2 was fabricated. Electrochemical performance for the LTO electrode with different porosities was comparatively studied. To achieve higher volume energy density, a gradient porous LTO electrode was prepared. As a result, the thick LTO electrode with a high mass loading of 20 mg cm–2 can deliver a high capacity of 150 mAh g–1 at 1 C with almost no ohmic drop under charge/discharge for 40 cycles.

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Summary Organic electrode materials have attracted extensive attention because of their high flexibility and sustainability, but their application was limited by the disadvantage of dissolution in conventional electrolyte. Here, we designed an all solid‐state lithium‐ion battery (ASSLIB) with 11,11,12,12‐tetracyano‐9,10‐anthraquinonedimethane (TCAQ) as the cathode and lithium metal as the anode. The solid electrolyte consisted of Li6.4La3Zr1.4Ta0.6O12 (LLZTO)/polyoxyethylene(PEO) and lithium bis(trifluoromethanesulfonimide) (LiTFSI) salt. The Li||TCAQ ASSLIB delivered a discharge specific capacity of 83 mAh g−1 at a current density of 17 mA g−1 with a capacity retention of 72.2% after 100 cycles. Our research provided a new organic cathode material for high‐performance ASSLIBs.