A unique MoS2-based composite composed of MoS2 nanosheets wrapped by a conductive polypyrrole (PPY) layer and closely incorporated within reduced graphene oxide (rGO) nanosheets is prepared by all-solution method. As a free-binder electrode for lithium-ion batteries, the ternary electrode delivers an initial discharge capacity of 1428 mAh g−1, maintains 1070 mAh g−1 after 400 cycles at a current density of 200 mA g−1, and also exhibits superior rate capacity of 600 mAh g−1 at a high current density of 2000 A g−1. The enhanced electrochemical performance is attributed to the advantageous combination of the 3D hierarchically rGO skeleton and in-situ formed conductive PPY coating. This design route represents a new direction for high-performance lithium ion batteries and related energy storage application with advanced nanostructured materials.