Free‐Standing Binder‐Free Cellulose‐Based MoS ₂ @C@CNFs Electrodes for Lithium–Sulfur Batteries

Lithium–sulfur (Li–S) batteries are promising high‐energy systems but suffer from the polysulfide shuttle effect, low sulfur conductivity, and large volume expansions. Herein, we report a novel, free‐standing, binder‐free sulfur host composed of hierarchical MoS 2 and carbon nanoparticle decorated cellulose‐based CNFs (MoS 2 @C@CNFs) for Li–S batteries for the first time. It is fabricated via electrospinning, carbon coating, carbonization, and hydrothermal methods. Carbon‐coated CNFs promote high active material loading and Li‐ion transport, while MoS 2 nanosheets anchored on C@CNFs further increase the surface area and provide abundant active sites. The hierarchical structure, consisting of 2D layered MoS 2 nanosheets and 0D carbon nanoparticles integrated onto the surface of 1D porous CNFs, creates a multiscale network that enhances reaction kinetics and electrical conductivity, mitigates the shuttle effect, and accommodates sulfur volume expansion. MoS 2 @C@CNFs cathode shows excellent electrochemical performance, delivering an initial capacity of 1320 mA h g −1 at 0.2C, and a reversible capacity of 1050 mA h g −1 after 250 cycles, with a capacity retention of 79.55%. After 450 cycles at 2C, it exhibits a low average capacity fading rate of 0.0885% per cycle. This study offers a novel strategy to produce free‐standing binder‐free cellulose‐based CNF electrodes for high‐performance Li–S batteries.