High-performance battery-type electrodes based on TiO2 nanotube arrays decorated with Co0·12Ni1·88S2@Co8S9 (CNCS) nanoparticles have been successfully prepared in this paper. The highly conductive TiO2 nanotube arrays modified with carbon and oxygen vacancies (Ti3+ defects) (m-TNAs) are selected as the three-dimensional backbones to support electroactive materials and offer direct pathways for electron and ions transport. Then CNCS nanoparticles are electrodeposited on each nanotube uniformly, and the loading mass of nanoparticles can be controlled through adjusting electrodeposition cycles. After optimization, a remarkable specific capacity of 680.1 C g−1 is achieved at 2 A g −1 as a result of the intrinsic synergetic contributions from structural/compositional/componental merits. This specific capacity is much higher than most of the TNAs-based energy storage electrodes. In addition, an asymmetric supercapacitor device is assembled by applying the optimized CNCS/m-TNAs and commercial active carbon as positive and negative electrode, respectively. It displays a high energy density of 45.5 Wh kg−1 at a power density of 400.5 W kg−1, after cycling for 3000 cycles at a high current density of 4 A g−1, the specific capacitance could still remain 85.7%. This self-supported and binder-free CNCS/m-TNAs electrode will be a competitive and promising candidate for the application in energy storage.