Herein, we report a convenient route to fabricate pseudohexagonal phase niobium pentoxide (TT-Nb 2 O 5 ) nanopillars via combination of laser ablation in liquids (LAL) and hydrothermal treatment without using any organic surfactants or stabilizers. The morphology and structure of the assynthesized samples are investigated through scanning and transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. Such nanopillars exhibit excel-lent lithium storage properties, including high reversible capacity, good rate capability, and excellent cycle stability (81% capacity retention after 1000 cycles) at a rate of 5 C in the potential range of 1.0 to 3.0 V, which is higher than other previously reported Nb 2 O 5 -based electrode. The synergistic effects from the nanopillar morphology, high electronic conductivity and stable structure promise potential applications in high-security and high-rate capability Li-ion batteries. Scheme 1. Schematic of the synthesis of TT-Nb 2 O 5 nanopillars.