Niobates with tungsten bronze crystal structures are regarded as prospective Li+-storage anode candidates due to the rich chemistry of niobium and structural openness. However, the exploration of this type of materials is still insufficient. Here, BiNb5.4O15 with a tetragonal tungsten bronze crystal structure (Cmmm space group) is explored. Abundant large-sized tunnels and a large interlayer spacing of ∼3.97 Å are found in this open structure, enabling fast Li+ diffusivity (3.25 × 10−11/1.68 × 10−10 cm2 ⋅ s−1 during lithiation/delithiation). Additionally, this structure is very stable after the first lithiation process, resulting in excellent cyclability (95.4%/∼100% capacity retention after 100/1000 cycles at 1C/10C). BiNb5.4O15 further exhibits a safe Li+-storage potential (∼1.55 V) and a large reversible capacity (309.7 mAh ⋅ g−1@ 0.1C). Therefore, BiNb5.4O15 can be a practical Li+-stora ge anode compound for large-scale energy-storage applications.