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SnO₂ nanoparticles (NPs) have been used as reversible high-capacity anode materials in lithium-ion batteries, with reversible capacities reaching 740 mAh·g⁻¹. However, large SnO₂ NPs do not perform well in charge–discharge cycling. In this work, we report the incorporation of MoS₂ nanosheet (NS) layers with SnO₂ NPs. SnO₂ NPs of ~5 nm in diameter synthesized by a facile hydrothermal precipitation method. Meanwhile, MoS₂ NSs of a few hundreds of nanometers to a few micrometers in lateral size were produced by top-down chemical exfoliation. The self-assembly of the MoS₂ NS layer on the gas–liquid interface was first demonstrated to achieve up to 80% coverage of the SnO₂ NP anode surface. The electrochemical properties of the pure SnO₂ NPs and MoS₂-covered SnO₂ NP anodes were investigated. The results showed that the SnO₂ electrode with a single-layer MoS₂ NS film exhibited better electrochemical performance than the pure SnO₂ anode in lithium storage applications.