A binder-free nano sulfur-carbon nanotube composite material featured by clusters of sulfur nanocrystals anchored across the superaligned carbon nanotube (SACNT) matrix is fabricated via a facile solution-based method. The conductive SACNT matrix not only avoids self-aggregation and ensures dispersive distribution of the sulfur nanocrystals but also offers three-dimensional continuous electron pathway, provides sufficient porosity in the matrix to benefit electrolyte infiltration, confines the sulfur/polysulfides, and accommodates the volume variations of sulfur during cycling. The nanosized sulfur particles shorten lithium ion diffusion path, and the confinement of sulfur particles in the SACNT network guarantees the stability of structure and electrochemical performance of the composite. The nano S-SACNT composite cathode delivers an initial discharge capacity of 1071 mAh g(-1), a peak capacity of 1088 mAh g(-1), and capacity retention of 85% after 100 cycles with high Coulombic efficiency (∼100%) at 1 C. Moreover, at high current rates the nano S-SACNT composite displays impressive capacities of 1006 mAh g(-1) at 2 C, 960 mAh g(-1) at 5 C, and 879 mAh g(-1) at 10 C.