Binders have been considered to play a key role in realizing high-energy-density lithium–sulfur batteries. However, the accompanying problems of limited conductivity and inferior affinity of soluble polysulfide intermediates bring down their comprehensive performance for practical applications. Herein, the synthesis of a novel double-chain polymer network (DCP) binder by polymerizing 4,4′-biphenyldisulfonic acid connected pyrrole monomer onto viscous sodium carboxymethyl cellulose matrix, yielding a primary crystal structure is reported. Consequently, the resulted binder enables superior rate performance from 0.2 C (1326.9 mAh g?1) to 4 C (701.4 mAh g?1). Moreover, a high sulfur loading of 9.8 mg cm?2 and a low electrolyte/sulfur ratio (5:1, μL mg?1) are achieved, exhibiting a high area capacity of 9.2 mAh cm?2. In situ X-ray diffraction analysis is conducted to monitor the structural modifications of the cathode, confirming the occurrence of sulfur reduction/recrystallization during charge–discharge process. In addition, in situ UV–vis measurements demonstrate that DCP binder impedes the polysulfide migration, thereby giving rise to high capacity retention for 400 cycles.
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