Significant effort has been made to explore high-performance anode materials for flexible lithium-ion batteries. We report a facile hydrothermal route to synthesis self-organized bunched akaganeite (β-FeOOH) nanorod arrays directly grown on carbon cloth (CC/β-FeOOH NRAs). Interestingly, the single nanorod is assembled by numerous small nanowires. A possible growth mechanism for this unique structure is proposed. Owning to the essential crystal structure of β-FeOOH (body-centered cubic), porous morphology, high surface area and direct growth on current collector, the prepared CC/β-FeOOH NRAs manifest a very high reversible capacity of ≈2840 mAh g−1 (2.21 mAh cm−2), remarkable rate capability 568 mAh g−1 (0.43 mAh cm−2) at 10C, stable cycling performance and greater mechanical strength.