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MoS 2 three dimensional (3D) architectures with various subunits were synthesized using glycerol to mediate the growth of MoS 2 crystals though a CS 2 -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 MoS 2 architecture, composed of nanosheets with a tiny size, ∼3 layers and expanded interlayer distance, namely MoS 2 -15, was obtained when the volume proportion of glycerol reaches 15%. The sample MoS 2 -15 exhibits superior electrochemical performance in lithium ion storage, due to reasonable design as well as smart organization of MoS 2 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 MoS 2 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. [ABSTRACT FROM AUTHOR]