Few‐Layer MoS ₂ –Decorated MoO ₂ for High‐Density Exposed Catalytic Heterointerfaces in Lithium–Sulfur Batteries

ABSTRACT Lithium–sulfur batteries are severely limited by polysulfide shuttling and sluggish sulfur redox kinetics. Efficient catalysis in lithium–sulfur (Li–S) batteries requires not only intrinsically active catalyst materials but also catalytic interfaces with high structural exposure and electrochemical accessibility. Here, a few‐layer MoS 2 –decorated MoO 2 composite integrated with carbon nanotubes is developed as a functional separator coating with a high density of exposed catalytic heterointerfaces. In this composite, polar MoO 2 strongly anchors lithium polysulfides, while highly dispersed few‐layer MoS 2 nanoflakes provide abundant MoO 2 –MoS 2 heterointerfaces, accelerating polysulfide conversion. Meanwhile, the MoO 2 –MoS 2 junction provides balanced polysulfide adsorption and pronounced charge redistribution, thereby promoting the activation and subsequent conversion of reaction intermediates. Li 2 S nucleation tests and in situ x‐ray diffraction further verify the accelerated kinetics of polysulfide conversion and the improved reversibility of Li 2 S formation. As a result, Li–S cells deliver a high specific capacity of 1236 mAh g −1 at 0.2 C and retain 475 mAh g −1 after 1000 cycles at 1 C, highlighting the promise of constructing high‐density exposed catalytic heterointerfaces for high‐performance Li–S batteries.