Lithium-sulfur (Li-S) batteries offer theoretical energy density much higher than that of lithium-ion batteries, but their development faces significant challenges. Mesoporous carbon-sulfur composite microspheres are successfully synthesized by combining emulsion polymerization and the evaporation-induced self-assembly (EISA) process. Such materials not only exhibit high sulfur-specific capacity and excellent retention as Li-S cathodes but also afford much improved tap density, sulfur content, and areal capacity necessary for practical development of high-energy-density Li-S batteries. In addition, when incorporated with carbon nanotubes (CNTs) to form mesoporous carbon-CNT-sulfur composite microspheres, the material demonstrated superb battery performance even at a high current density of 2.8 mA/cm(2), with a reversible capacity over 700 mAh/g after 200 cycles.