Ultrathin MoS2 nanosheets were prepared in high yield using a facile and effective hydrothermal intercalation and exfoliation route. The products were characterized in detail using X-ray diffraction, scanning electron microscopy, transmission electron microscopy and Raman spectroscopy. The results show that the high yield of MoS2 nanosheets with good quality was successfully achieved and the dimensions of the immense nanosheets reached 1 μm–2 μm. As anode material for Li-ion batteries, the as-prepared MoS2 nanosheets electrodes exhibited a good initial capacity of 1190 mAh·g−1 and excellent cyclic stability at constant current density of 50 mA·g−1. After 50 cycles, it still delivered reversibly sustained high capacities of 750 mAh·g−1.