In this work, three different morphologies of CuCo2S4 materials have been prepared by a facile hydrothermal synthesis route by controlling the species of solvent and molar concentration of precursors. The effects of reaction conditions on the physical characteristics (including microstructure, morphology, specific surface area and pore structure) and electrochemical behaviors of the products were systematically investigated. The experimental results reveal that as-obtained highly uniform micro-/nanostructure CuCo2S4 particles prepared by mixed solvent (H2O/ethylene glycol(EG)) and low molar concentration of precursors manifest the best electrochemical performances. The specific capacity is up to 90.6mAhg−1 at a current density of 2Ag−1, and 47.9% of capacity retention rate can be retained when the current density varies from 2 to 50Ag−1. Furthermore, a superior cycling stability with 95.6% of initial capacity retention rate can be maintained at 3Ag−1 after 5000 consecutive charge-discharge cycles. The enhanced electrochemical performances can be mainly attributed to the highly uniform micro-/nanostructure with relatively larger specific surface area and total pore volume. Therefore, the results above demonstrate that the as-prepared highly uniform micro-/nanostructure CuCo2S4 particles might be promising candidate battery electrode materials for energy storage.