3D composites of layered MoS₂ and interconnected graphene nanoribbons (GNRs) are synthesized by a facile one-pot hydrothermal method. During the synthesis process, the GNRs self-assemble into conductive bridges between the MoS₂ layers to form 3D structures that exhibit large specific capacity, good cycling stability and rate capability. Specifically, the composites exhibit a specific capacity of 1009.4 mA h g⁻¹ at 200 mA g⁻¹ after 80 cycles of the cycling test. They also exhibit a specific capacity of 606.8 mA h g⁻¹ at 3 A g⁻¹ in the rate capability test. In comparison, the bare MoS₂ nanoparticles exhibit a specific capacity of 139.8 mA h g⁻¹ at 200 mA g⁻¹ after 80 cycles of the cycling test and 37.4 mA h g⁻¹ at 3 A g⁻¹ in the rate capability test. The structure, morphology and chemical analysis show that the superiority of the 3D structure is due to the large surface area and abundant mesopores that render a high contact area between the electrode and electrolyte. Moreover, the synergistic effects between the 2D MoS₂ layers and the 1D GNRs within the 3D structures enable fast Li ion and electron transportation, inhibit the self-aggregation of MoS₂ nanosheets, and accommodate the volume expansion to gain cycling stability and rate capacity.