Large-scale aligned CuO nanosheets on conductive carbon cloth were successfully synthesized by a facile two-step approach include magnetron sputtering and solution immersion. The in-situ growth mechanism for the CuO nanostructures is proposed. When tested as anodes for lithium-ion batteries, the CuO nanosheets delivers an initial capacity of 711.2mAhg−1 at 500mAg−1 and maintained 88% after 100 cycles. Even at 2000mAg−1, a stable capacity as high as 448.9mAhg−1 could be achieved. The obtained high performance is due to (1) 2D sheet-like structure with short diffusion length, fast electron transfer and efficient accommodation of volume expansion (2) carbon cloth substrate with high flexibility and conductivity (3) intermediate copper layer with enhanced mechanism adhesion (4) 3D hierarchical structure with large contact area between active material and electrolyte. Achieved electrochemical performance by directly growing ordered CuO nanosheets on conductive carbon cloth makes them promising anode for flexible LIB application.