Core-shell structure of ultrathin MoS2 nanosheets attached on carbon microspheres ([email protected]2) are synthesized through a simple and rapid L-cysteine-assisted hydrothermal procedure. When used as a promising anode for lithium ion battery, the as-synthesized [email protected]2 core-shell microspheres electrodes exhibit high capacity (1333 mAh g−1 of the first cycle and 753 mAh g−1 after 50 cycles at 0.2 A g−1), excellent rate capability (a reversible capacity of 850 mAh g−1 when the current density returns from 1600 to initial 100 mA g−1), and long cycling stability (a reversible capacity of 737 mAh g−1 after 200 cycles at a much higher current density of 1 A g−1). The superior electrochemical performances of [email protected]2 core-shell microstructures should be attributed to the purposely designed unique structures, in which the ultrathin 2D MoS2 nanosheets provide more lithium storage sites and shorter Li-ion diffusion length, and the micron-sized carbon microspheres maintain the structural integrity and improve the conductivity of active materials.