Much attention has recently been focused on the synthesis and application of graphene analogues of layered nanomaterials owing to their better electrochemical performance than the bulk counterparts. We synthesized graphene analogue of 3D MoS2 hierarchical nanoarchitectures through a facile hydrothermal route. The graphene-like MoS2 nanosheets are uniformly dispersed in an amorphous carbon matrix produced in situ by hydrothermal carbonization. The interlaminar distance between the MoS2 nanosheets is about 1.38 nm, which is far larger than that of bulk MoS2 (0.62 nm). Such a layered architecture is especially beneficial for the intercalation and deintercalation of Li+. When tested as a lithium-storage anode material, the graphene-like MoS2 hierarchical nanoarchitectures exhibit high specific capacity, superior rate capability, and enhanced cycling performance. This material shows a high reversible capacity of 813.5 mAh g−1 at a current density of 1000 mA g−1 after 100 cycles and a specific capacity as high as 600 mAh g−1 could be retained even at a current density of 4000 mA g−1. The results further demonstrate that constructing 3D graphene-like hierarchical nanoarchitectures can effectively improve the electrochemical performance of electrode materials.