Hierarchical Bi2MoO6 nanosheet arrays (BNAs) growing on three-dimensional (3D) Ni foam are synthesized by one-step template-free route. The obtained BNAs are used as binder-free integrated electrode for Li-ion batteries (LIBs) directly. The electrode exhibits a super high reversible discharge capacity of 2311.7[Formula: see text][Formula: see text]Ah[Formula: see text]cm[Formula: see text] (1741.4[Formula: see text]mAh[Formula: see text]g[Formula: see text]), and an excellent cycle stability. The outstanding electrochemical properties are reasonable from the self-supported integrated electrode in which the electrolyte is easy to infiltrate active materials, electrons and ions are readily transported along the 3D conductive substrate and the stable electrode structure.