Supercapacitors (SCs) are attractive as promising energy storage devices because of their distinctive attributes, such as high power density, good current charge/discharge ability, excellent cyclic stability, reasonable safety, and low cost. Electrode materials play key roles in achieving excellent performance of these SCs. Among them, binary transition metal sulfides (BTMSs) have received significant attention, attributed to their high conductivity, abundant active sites, and excellent electrochemical properties. This topic review aims to summarize recent advances in principles, design, and evaluation of the electrochemical performance for nanostructured BTMSs (including nickel–cobalt sulfides, zinc–cobalt sulfides, and copper–cobalt sulfides.) and their nanocomposites (including those carbon nanomaterials, transition metal oxides, binary transition metal oxides, transition metal sulfides, and polymers). Nanostructuring of these BTMSs and nanocomposites as well as their effects on the performance were discussed, including nanoparticles, nanospheres, nanosheets, nanowires, nanorods, nanotubes, nanoarrays, and hierarchitectured nanostructures. Their electrochemical performance has further been reviewed including specific capacitance, conductivity, rate capability, and cycling stability. In addition, the performance of hybrid supercapacitors (HSCs) assembled using the nanostructured BTMSs as the cathodes also have been summarized and compared. Finally, challenges and further prospects in the HSCs-based BTMS electrodes are presented.