A series of PANI-CNTs/TiO2 nanotubes/Ti electrodes were fabricated via pulse current co-electrodeposition of polyaniline and functionalized carbon nanotubes onto TiO2 nanotubes/Ti electrodes. FT-IR spectrometry, X-ray photoelectron spectroscopy, and scanning electron microscopy were applied in order to characterize the modified TiO2 nanotubes/Ti electrodes. The morphology studies showed that the PANI-CNTs/TiO2 nanotubes/Ti nanocomposite electrode has many interlaced PANI-CNTs nanorods on the surface of TiO2 nanotubes. The electrochemical measurements of the modified electrodes confirmed that the CNTs in the composite can significantly improve the capacitive behavior as well which have been compared with that of PANI/TiO2 nanotubes/Ti electrodes. The modified electrode exhibited much higher specific capacitance (190 mF cm−2 with 90% retention after 1000 cycles) compared to the PANI/TiO2 nanotubes/Ti (70 mF cm−2 with 77% retention after 1000 cycles) at a current density of 0.85 mA cm−2, indicating its great potential for supercapacitor applications.