Uniform nanocable-like Nb2O5/surface-modified carbon nanotubes (SMCNTs) composites for anode materials in lithium ion batteries were synthesized by hydrothermal method. It was indicated that Nb2O5 nanoparticles were tightly and uniformly cultivated on carbon nanotubes when CNTs were pretreated with concentrated H2SO4. As a result, Nb2O5/SMCNTs composite materials showed remarkable electrochemical performance as anode materials for lithium-ion batteries. It delivered a high reversible capacity of 441mA h g−1 cycled at the current density of 40mAg−1 after 100 cycles and an excellent rate capacity of 185mA h g−1 at the high current density of 5000mAg−1 after 200 cycles.