The controllable construction of two-dimensional (2D) metal–organic framework (MOF) nanosheets with favorable electro-chemical performances is greatly challenging for energy storage. Here, we design an in situ induced growth strategy to construct the ultrathin carboxylated carbon nanotubes (C-CNTs) interpenetrated nickel MOF (Ni-MOF/C-CNTs) nanosheets. The deliberate thickness and specific surface area of novel 2D hybrid nanosheets can be effectively tuned via finely controlling C-CNTs involvement. Due to the unique micro-structure, the integrated 2D hybrid nanosheets are endowed with plen-tiful electroactive sites to promote the electrochemical performances greatly. The prepared Ni-MOF/C-CNTs nanosheets exhibit superior specific capacity of 680 C g-1 at 1 A g-1 and good capacity reten-tion. The assembled hybrid device demonstrated the maximum energy density of 44.4 Wh kg-1 at a power density of 440 W kg-1. Our novel strategy to construct ultrathin 2D MOF with unique properties can be extended to synthesize various MOF-based functional materials for diverse applications.