MoS2 three dimensional (3D) architectures with various subunits were synthesized using glycerol to mediate the growth of MoS2 crystals though a CS2-assisted hydrothermal approach. It has been found that the thickness and lateral size of subunits can be distinctly reduced by increasing glycerol content in the mixture solvent. A stable porous MoS2 architecture, composed of nanosheets with a tiny size, similar to 3 layers and expanded interlayer distance, namely MoS2-15, was obtained when the volume proportion of glycerol reaches 15%. The sample MoS2-15 exhibits superior electrochemical performance in lithium ion storage, due to reasonable design as well as smart organization of MoS2 subunits, featured by a capacity of 1027 mAh g(-1) at 0.1 A g(-1) after 100 cycles and 738 mAh g(-1) at 5 A g(-1) after 300 cycles, exceeding other MoS2 nanostructured materials in this work. More importantly, the as-prepared various architectures exhibit tunable electrochemical behaviors depending on structure and morphology evolution, which truly reflects the potential to optimize the microstructure for lithium-ion host materials.