Li-S batteries benefit from numerous advantages such as high theoretical capacity, high energy density, and availability of an abundance of sulfur. However, commercialization of Li-S batteries has been impeded because of low loading amount of active materials and poor cycle performance. Herein, a freestanding bilayer carbon-sulfur (FBCS) cathode is reported with superior electrochemical performance at a high sulfur loading level (3 mg cm(-2)). The top component of the FBCS cathode is composed of interlacing multiwalled carbon nanotubes (MWCNT) and the bottom component is made up of a mixed layer of sulfur imbedded in MWCNT and N-doped porous carbon (NPC). The MWCNT layer (top part of FBCS cathode) blocks polysulfide migration from the cathode to the anode, and NPC in the bottom part of the FBCS cathode not only provides spacious active sites but also absorbs polysulfide by the nitrogen functional group. The designed novel FBCS cathode delivered a high initial discharge capacity of 964 and 900 mAh g(-1) at 0.5 and 1 C, respectively. It also displayed an excellent capacity retention of 83.1% at 0.5 C and 83.4% at 1 C after 300 cycles.