2666 wileyonlinelibrary.com charger mobility, and the others. [ 7,8 ] These properties have made graphene be one of the most promising materials in the 21st century for supercapacitors, [ 9,10 ] Li-ion batteries, [ 11,12 ] and fuel cell. [ 13,14 ] Apart from graphene, other 2D nanomaterials have also been regarded as attractive materials recently, such as transition-metal dichalcogenides (TMDs), [15][16][17] layered double hydroxides, [18][19][20] transition metal oxide nanosheets, [21][22][23] and graphene analogues. [ 24 ] In addition, a variety of 2D composites with novel structures and exceptional properties were developed for high technology applications.MoS 2 with a sandwich interlayer structure is a typical TMD, which is formed by a stack of planes. Each plane is composed of covalently bonded three atom (S-Mo-S) layers, and adjacent planes are held together by weak van der Waals interactions. MoS 2 nanosheets with single layer or few layers exhibit unexpectedly exotic behaviors compared with the bulk MoS 2 . A few new strategies have been developed for the synthesis of MoS 2 nanosheets, such as modifi ed liquid exfoliation, [ 25 ] hydrothermal or solvothermal synthesis, [ 26,27 ] and laser thinning. [ 28 ] However, the MoS 2 nanosheets are easily agglomerated for high surface energy, which leads to serious decrease of the performance. One of effective solutions is dispersing the nanosheets on the support materials, [ 29 ] such as graphene, [30][31][32] carbon nanotubes, [ 33 ] and TiO 2 [ 34,35 ] . MoS 2 composites exhibit excellent performance in hydrogen evolution reaction, [ 36 ] lithium ion storage, [ 37 ] and catalysis, which could be attributed to the support of matrix materials. The effects of matrix materials for enhancing properties of MoS 2 composites are mainly preventing the agglomeration of MoS 2 , exposing active edge sites, providing electronic transmission channel and promoting the separation of photoelectrons from vacancies. However, the interfacial structure between MoS 2 and matrix materials requires further investigation.Montmorillonite (MMT) is one of the most abundant nature clay mineral with 2D sheet-like morphology. The montmorillonite sheets consist of three layer structural units (TOTs), which are composed of a central AlO 4 (OH) 2 octahedral sheet and two SiO 4 tetrahedral sheets. It is a promising matrix material for assembling nanoparticles for its 2D sheet-like morphology, large specifi c surface area, and abundant hydroxyl groups. Montmorillonite has also been successfully used to