The structural design and synthesis of sulfur-carbon composite materials with high performance is still a major challenge for rechargeable lithium-sulfur batteries. Interconnected three-dimensional frameworks comprising multi-walled carbon nanotubes, graphene, or carbon particles offer a combination of constituent advantages and can thus be used to achieve superior energy conversion and storage properties. Herein, we designed and prepared free-standing three-dimensional sulfur papers containing interconnected highly conductive carbon materials, which enable to be flexible binder-free cathodes for Li-S batteries. The resultant sulfur-carbon composite paper cathode exhibited high reversible specific capacity of 1386 mAhg−1, good rate capability up to 5C, and excellent cycling performance (a capacity retention 68% after 400 cycles), all of which are significantly improved from those of bare sulfur cathode or sulfur-GO composite only. Rational design of cathode composition, structure, and a simple fabrication process can give insight into the development of various advanced cathode materials for high-performance Li-S batteries.