Lithium-sulfur batteries attract much interest as energy storage devices for their low cost, high specific capacity, and energy density. However, the insulating properties of sulfur and high solubility of lithium polysulfides decrease the utilization of active materials by the battery resulting in poor cycling performance. Herein, we design a multifunctional carbon-nanotube paper/titanium-dioxide barrier which effectively reduces active material loss and suppresses the diffusion of lithium polysulfides to the anode, thereby improving the cycling stability of lithium-sulfur batteries. Using this barrier, an activated carbon/sulfur cathode with 70% sulfur content delivers stable cycling performance and high Coulombic efficiency (~99%) over 250 cycles at a current rate of 0.5 C. The improved electrochemical performance is attributed to the synergistic effects of the carbon nanotube paper and titanium dioxide, involving the physical barrier, chemical adsorption from the binding formation of Ti-S and S-O, and other interactions unique to the titanium dioxide and sulfur species.