As promising, safe, high-power electrode materials for lithium-ion batteries (LIBs), titanium-dioxide-based anodes that have been prepared to date are still restricted by their limited specific capacity. In this work, we demonstrate a facile electrochemical anodization for TiOx nanotubular arrays of oxygen defects in a nitrogen atmosphere. In comparison with those fabricated under air conditions, the as-prepared nanotubular arrays present much reduced impedance with oxygen defects, which allow fast electronic and ionic transport in the TiOx nanotubular arrays. The binder-free anode based on as-prepared TiOx nanotubular arrays exhibited record-setting capacities (395, 325, and 235 mAh g−1 at 0.2, 1, and 10 C, respectively) among TiO2-based anode materials, that is, approaching state-of-the-art TiO2 electrodes for LIBs.