Mullite-type compound Bi 2 Mn 4 O 10 has shown the feasibility as anodes of next lithium-ion batteries (LIBs). Herein micro/nano-Bi 2 Mn 4 O 10 with hierarchical spindle-like architectures has been successfully synthesized using a one-step hydrothermal method without any no surfactant or template. A time-dependent experiment is carried out to observe the morphology evolution, suggesting a nucleation-aggregation/growth-dissolution-recrystallization process. As anode of LIBs, the as-prepared spindle-shaped micro/nano Bi 2 Mn 4 O 10 harvests a significantly high initial discharge capacity of 1022 mA h g −1 at 1 C, an excellent cyclability performance (563.8 mA h g −1 after 400 cycles), a better high-rate capability (100 mA h g −1 at 10 C), quick diffusion kinetics (1.8 × 10 −12 cm 2 s −1 ), and low active energy (19.5 kJ mol −1 ), which are significantly superior to that of its bulk counterparts and the previous reports. The encouraging lithium storage performance largely stems from the synergistic effect of the unique spindle-shaped micro/nanostructure.