The sulfur redox in Li–S batteries involves a complex sequence of solid–liquid–solid conversions, and reaction catalysis has recently become a focused area for further advancement. The deposition of solid Li2S from liquid Li2S4 contributes to three-quarters of the total theoretical capacity and is therefore of great significance over the entire cathode reaction. This study demonstrates a cathode material composed of carbon nanofibers decorated with catalytic Co phthalocyanine nanorods (CoPc@CNF), which are highly effective in promoting the deposition of Li2S in three-dimensional (3D) fine particles rather than 2D thin films. This significantly alleviates cathode passivation during cell charge and discharge, leading to obviously improved sulfur utilization and cycling stability for high loading cathodes. DFT calculations indicate that the promoted 3D deposition of Li2S is related to the facilitated migration of deposition precursors (Li2S4 and Li-ions) to migrate on the CoPc nanorods. Lithium–sulfur (Li–S) pouch cells were prepared with high specific (954 mAh g–1), areal (4.8 mAh cm–2), and total (235 mAh) capacities achieved at 0.5 C under high sulfur content. As metal phthalocyanines possess a high structural variability, this study provides opportunities to the design of a new class of Li–S cathode materials.

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