Lithium sulfide (Li2S) is an attractive cathode material with a high theoretical specific capacity (1166 mAh g(-1)). However, the poor cycle life and rate capability have remained significant challenges, preventing its practical application. Here, Li2S spheres with size control have been synthesized for the first time, and a CVD method for converting them into stable carbon-coated Li2S core-shell (Li2S@C) particles has been successfully employed. These Li2S@C particles with protective and conductive carbon shells show promising specific capacities and cycling performance with a high initial discharge capacity of 972 mAh g(-1) Li2S (1394 mAh g(-1) S) at the 0.2C rate. Even with no added carbon, a very high Li2S content (88 wt % Li2S) electrode composed of 98 wt % 1 μm Li2S@C spheres and 2 wt % binder shows rather stable cycling performance, and little morphology change after 400 cycles at the 0.5C rate.