of using molecular hydrogen (H 2) as carbon-free fuel produced by renewable energy sources. [2] To embrace H 2 as game changer, academic research is struggling to develop advanced electrolysers, while reducing their investment and operational costs. [3] In this context, proton exchange membrane (PEM) water electrolysers overcome several operational drawbacks of commercial alkaline ones, [4] for example, low maximum achievable current density (between 200 and 400 mA cm −2), low operating pressure (<30 bar), inefficient dynamic operation (acceptable part-load operation between 10 and 40% of the nominal load), and gas crossover phenomena (typical gas purity <99.9%). [3,5] Nonetheless, the costs and the scarcity of their most effective catalysts, for example, Pt-group elements for the hydrogen evolution reactions (HER) at the cathode, [6,7] and RuO 2 /IrO 2 for the oxygen evolution reactions at the anode, [8,9] hinder massive commercial products. [10] To face the cost-related barriers of the PEM electrolysers, it is mandatory to search for alternative nonprecious catalysts, [11,12] or at least to reduce the content of precious metals, while still maintaining the electrochemical The nanoengineering of the structure of transition metal dichalcogenides (TMDs) is widely pursued to develop viable catalysts for the hydrogen evolution reaction (HER) alternative to the precious metallic ones. Metallic group-5 TMDs have been demonstrated to be effective catalysts for the HER in acidic media, making affordable real proton exchange membrane water electrolysers. Their key-plus relies on the fact that both their basal planes and edges are catalytically active for the HER. In this work, the 6R phase of TaS 2 is "rediscovered" and engineered. A liquid-phase microwave treatment is used to modify the structural properties of the 6R-TaS 2 nanoflakes produced by liquid-phase exfoliation. The fragmentation of the nanoflakes and their evolution from monocrystalline to partly polycrystalline structures improve the HER-activity, lowering the overpotential at cathodic current of 10 mA cm −2 from 0.377 to 0.119 V. Furthermore, 6R-TaS 2 nanoflakes act as ideal support to firmly trap Pt species, which achieve a mass activity (MA) up 10 000 A g Pt −1 at overpotential of 50 mV (20 000 A g Pt −1 at overpotentials of 72 mV), representing a 20-fold increase of the MA of Pt measured for the Pt/C reference, and approaching the state-of-the-art of the Pt mass activity.