In this work, 3D hierarchical flower-like MoS2 spheres are successfully fabricated via a hydrothermal method followed by a heat treatment. The obtained product is composed of few-layered MoS2 nanosheets with enlarged interlayer distance (ca. 0.66 nm) of the (002) plane. Meanwhile, the hydrogen storage properties of the as-prepared MoS2 ball milled with LiBH4 are systematically investigated. The results of temperature programmed desorption (TPD) and isothermal measurement suggest that the LiBH4-MoS2 (as-prepared) mixture exhibits favorable dehydrogenation properties in both lowering the hydrogen release temperature and improving kinetics of hydrogen release rate. LiBH4-MoS2 (as-prepared) sample (the preparation mass ratio is 1:1) starts to release hydrogen at 171 degrees C, and roughly 5.6 wt % hydrogen is released within 1 h when isothermally heated to 320 degrees C, which presents superior dehydrogenation performance compared to that of the bulk LiBH4. The excellent dehydrogenation performance of the LiBH4-MoS2 (as-prepared) mixture may be attributed to the high active site density and enlarged interlayer distance of the MoS2 nanosheets, 3D architectures and hierarchical structures. (C) 2015 Elsevier B.V. All rights reserved.