Although various methods have been developed to disperse transition metal dichalcogenides (TMDCs) in aqueous environments, the methodology to generate stable TMDC dispersions remains challenging. Here, we developed a hierarchical van der Waals (vdW) heterostructure-based strategy to disperse few-layered TMDCs (WS 2 , MoS 2 , WSe 2 , and MoSe 2 ) using both hexagonal boron nitride (hBN) and sodium cholate (SC) as synergistic vdW surfactants. By showing long-term stability of up to 3 years, the extinction spectra of these TMDC/hBN/SC dispersions exhibit the most blue-shifted excitonic transitions, low background extinction, good colloidal stability, and dispersion stability upon ultracentrifugation compared to other dispersion methods. Hierarchical stacking having TMDCs and hBN/SC as core and shell parts is probed by electrostatic/atomic force microscopy and zeta potential, and its origin was attributed to surface energy matches. Along with the synergetic effect between TMDCs and hBN, the blue shift was ascribed to compressive strain on the TMDCs caused by hBN wrapping. The results of transmission electron microscopy show that the TMDCs in the dispersions have defective, few-layered structures with flake sizes that are less than a few hundred nm 2 . Raman spectroscopy is used to study not only the existence of compressive strain but also various interlayer coupling between TMDC and hBN. The hierarchical structures of TMDC/hBN/SC are discussed in terms of surface energies and topographies. This method is invaluable to provide a general methodology to disperse various surface-corrugated dimensional materials for various dispersion-based applications.
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