Molybdenum disulfide (MoS2) has emerged as a promising anode material for lithium-ion batteries (LIBs), but its practical application is limited by poor cycling stability and low rate capability. Herein, we propose a facile mesopore-confined growth approach to synthesize 3D ordered, graphene-supported, highly curved MoS2 frameworks (named MoS2@OMGSs) for superior lithium-ion storage. The graphene-encapsulated and highly curved MoS2 leads to enhanced cycling stability. Meanwhile, the ordered mesoporous superstructures of carbon hosts enable fast electron and ion transport, resulting in excellent rate capability. Specifically, MoS2@OMGSs displays high specific capacities of 1350 and 400 mAh g−1 at current densities of 0.1 and 10 A g−1, respectively, along with excellent cycling stability of 500 cycles at 1.0 A g−1. The work paves the way for further development of well-defined electrode materials for high-performance LIBs.