LAUSR

The lack of highly efficient, durable, and cost‐effective electrocatalysts for the hydrogen evolution reaction (HER) working at high current densities poses a significant challenge for the large‐scale implementation of hydrogen production from renewable energy. Herein, amorphous molybdenum tungsten sulfide/nitrogen‐doped reduced graphene oxide nanocomposites (a‐MoWSx/N‐RGO) are synthesized by plasma treatment for use as high‐performance HER catalysts. By adjusting the plasma treatment duration and chemical composition, an optimal a‐MoWSx/N‐RGO catalyst is obtained, which exhibits a low overpotential of 348 mV at a current density of 1000 mA cm−2 and almost no decay after 24 h of working at this current density, outperforming commercial platinum/carbon (Pt/C) and previously reported heteroatom‐doped MoS2‐based catalysts. Based on density functional theory (DFT) calculations, it is found that with a reasonable tungsten doping level, the catalytic active site (2S2 − ) shows excellent catalytic performance working at high current densities because extra electrons preferentially fill at 2S2 − . The introduction of tungsten tends to lower the electronic structure energy, resulting in a closer‐to‐zero positive ΔGH∗$\Delta {G}_{{{\rm{H}}}^{\rm{*}}}$ . Excessive tungsten introduction, however, can lead to structural damage and a worse HER performance under high current densities. The work provides a route towards rationally designing high‐performance catalysts for the HER at industrial‐level currents using earth‐abundant elements.