Transition metal dichalcogenides (TMDs) have recently emerged within the group of 2D materials due to their electrical, catalytic and optical properties significantly enhanced and useful when down-sized to single layer.I n particular,MoS 2 has attracted much attention due to its semiconducting nature with au seful band gap when presenta s single layer,t he enhanced photoluminescence, but also importantly the excellent catalytic properties towards the electrochemical hydrogen evolution. We present heret he preparation of thin layers MoS 2 nanosheetsw ith enhanced catalytic properties towards the hydrogen evolution reaction by meanso fa ne asy and fast electrochemical top-down exfoliation procedurei na queous solution from an aturally occurring MoS 2 crystal. After structurala nd chemical characterization with STEM, AFM, XPS and Raman spectroscopy electrochemicali nvestigationsw ere performed to test catalytic properties in acidic solution for the electrogeneration of hydrogen and compare it to MoS 2 nanosheets obtained through the widelye mployed chemical Li intercalation/exfoliation. Electrochemically exfoliated MoS 2 shows lower Ta fel slope than its counterparto btainedw ithc hemical exfoliation.[a] Dr.A .Ambrosi, Prof. Dr.M .P umera DivisionofChemistry &B iological Chemistry SchoolofP hysical and Mathematical SciencesSupporting information containing STEM images of chemically exfoliated MoS 2 and XPS survey spectra of chemically and electrochemically exfoliated MoS 2 ,and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.