In summary, α-MoO3 nanobelts with smooth surface and uniform thickness have been synthesized via a hydrothermal method, and the electrodes exhibited good Li+ storage performance, which demonstrated a high specific capacity of 900 mA h g−1 maintained after 60 cycles at 0.2 A g−1, and even keeping 480 mA h g−1 when the current density increased to 2 A g−1. Therefore, α-MoO3 nanobelts could be a promising candidate for high power LIBs.