Self-assembled Cu-Co-S nanosheets with hierarchical structure have been obtained by means of a gelation-solvothermal process without using any surfactant or template and utilized as anode materials in lithium-ion batteries. The Cu-Co-S nanosheets display a reversible high specific capacity of 1045.1 mAh g(-1) after 100 cycles at 200 mA g(-1) and retaining a reversible specific charge capacity of 510.7 mAh g(-1) after 500 cycles at 1 A g(-1) with a retention of 94.5%. Combining the hierarchical structure with the unique chemical composition, synergetic merits are noticed. The improved electric conductivity, shortened Li+ diffusion length and increased electrolytes penetration areas are achieved synchronously, giving rise to significant high capability and extraordinary cycling stability.