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Orthorhombic α‐MoO3 is a potential anode material for lithium‐ion batteries due to its high theoretical capacity of 1100 mAh g−1 and excellent structural stability. However, its intrinsic poor electronic conductivity and high volume expansion during the charge–discharge process impede it from achieving a high practical capacity. A novel composite of α‐MoO3 nanobelts and single‐walled carbon nanohorns (SWCNHs) is synthesized by a facile microwave hydrothermal technique and demonstrated as a high‐performance anode material for lithium‐ion batteries. The α‐MoO3/SWCNH composite displays superior electrochemical properties (654 mAh g−1 at 1 C), excellent rate capability (275 mAh g−1 at 5 C), and outstanding cycle life (capacity retention of >99% after 3000 cycles at 1 C) without any cracking of the electrode. The presence of SWCNHs in the composite enhances the electrochemical properties of α‐MoO3 by acting as a lithium storage material, electronic conductive medium, and buffer against pulverization.

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