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The catalysis of covalent organic frameworks (COFs) in Li–S chemistry is largely blocked by a weak chemical interaction and low conductivity. Herein, a new kind of diketopyrrolopyrrole (DPP)-based COF is in situ fabricated onto the carbon nanotube (CNT) surface (denoted as COF@CNT) to uncover the electrocatalysis behavior by its strong chemical interaction and highly conductive property. We declare that the electrocatalytic activity of DPP-COF can be maximized by introducing an appropriate content of CNT (66 wt %); the analyses including density functional theory calculations, X-ray photoelectron spectroscopy, Fourier transform infrared, and Raman show that the DPP moiety can mediate the conversion of polysulfides contributed by a C═O/C–O bonding conversion. Hence, the modified battery shows a 0.042% decay rate over 1000 cycles and achieves a desirable capacity of 8.7 mAh cm^–2 with 10 mg cm …