Three-dimensional (3D) interwoven nitrogen-doped carbon nanotubes (N-CNTs)/CoxNi1-x-layered double hydroxides (CoxNi1-x-LDHs) ultrathin nanosheets on Ni foam have been rationally designed via the combination of chemical vapor deposition and electrochemical deposition approaches. The CoxNi1-x-LDHs nanosheets are uniformly distributed on the N-CNTs, which can not only serve as the stable frame to improve the specific surface area, but also can enhance the conductivity. The Ni foam/N-CNTs/Co0.5Ni0.5-LDHs nanosheets electrode displays a remarkable maximum capacitance (2170Fg−1 at 1Ag−1 and 1.62Fcm−2 at 1mAcm−2), excellent rate capability (80.9% specific capacitance retention at 20Ag−1 and 75.8% areal capacitance retention at 30mAcm−2) and good cycling stability. First-principles calculations further reveal that the Co doping can effectively reduce the band gap of Ni(OH)2 and increase the conductivity. This work demonstrates a facile synthesis strategy of 3D hierarchical Ni foam/N-CNTs/CoxNi1-x-LDHs nanosheets electrode with remarkable electrochemical properties, which can be used in energy storage and conversion.