Nickel-cobalt organic framework (denoted as NiCo-MOF) nanosheet assemblies are prepared through a controllable one-pot hydrothermal synthesis procedure at 150 °C. The as-prepared samples are directly employed as electrode materials for electrochemical energy storage (EES), and exhibit excellent electrochemical performance. Among these samples, NiCo-MOF-1 displays a high capacity of 100.18 mA h g-1 (901.60 F g-1), and obtains a capacity retention of 81.00% over 3000 cycles at 5 A g-1. Likewise, in an aqueous device, NiCo-MOF-1//AC delivers a discharge capacity of 83.75 mA h g-1, and also exhibits a good cycling life (74.14% retention after 3000 cycles). These results demonstrate that multilayer NiCo-MOF nanosheet assemblies are potential electrode materials for EES.