Carbon nanotubes (CNTs) grown on the carbon fiber paper (CFP) via chemical vapor deposition system is used as flexible substrate. NiO nanoparticles are electrodeposited onto CNTs/CFP flexible substrate by electrochemical deposition technique, which is used as a flexible electrode for supercapacitors. The NiO@CNTs/CFP electrode displays specific capacitance as high as 1317 F g -1 at a current density of 1.2 A g -1 , which can preserve a capacitance retention of 90.6 % with a high current density of 9.6 A g -1 . After 3000 cycles, the composite electrode can retain 90 % of initial capacitance, showing good cyclability. Meanwhile, the 3D porous nanostructure of NiO@CNTs/CFP electrode can offer a great opportunity to fabricate a high-performance flexible binder-free supercapacitor electrode, in which all of the materials could take part in the charge-storage process with their surface in direct contact with the electrolyte.