Hydrogen evolution reaction (HER) is a vital step for electrochemical energy conversion technologies. However, developing cost-efficient electrocatalysts remains a huge challenge. Here, we report that Cr-doped NiSx (Cr-NiSx) in situ grown on Ni foam via a hydrothermal sulfurization reaction can be an ultra-highly efficient and low-cost electrocatalyst for HER in alkaline condition. We find that the Cr-doping can trigger the formation of NiS and NiS1.19, leading to the suppression of Ni3S2 in the nanostructure. We show that Cr-NiSx exhibits an excellent HER activity with an ultralow overpotential of 81 mV at 10 mA cm−2, better than those of most nickel sulfide catalysts, and good stability. Our combined experimental and computational study reveals that the excellent performance is contributed by: (1) stabilized NiSx phase, (2) strongly improved conductivity, (3) greatly enhanced active sites, and (4) reduced Gibbs free energy for hydrogen adsorption (ΔGH) due to the Cr-doping. We believe that this work provides a simple approach to design cost-effective and ultra-highly efficient HER electrocatalysts for practical applications.