A new pretreatment method has been developed to improve the catalytic activity of the Ni-Fe-Mo-Co alloy elec- trode for hydrogen evolution reaction (HER). The procedure involves pre-electrolyzing the Ni-Fe-Mo-Co alloy electrode in 30% KOH solution containing 10% potassium sodium tartrate at 70°C for 2 h, until some of the Mo and Fe elements are leached out. The surface morphology of the Ni-Fe-Mo-Co alloy demonstrates a unique hive-like structure after the pre- treatment, which has the pore size in a nanometer range (about 50 nm), a very large real surface area, and good stability. The results of the electrochemical studies show that compared to other similar electrode materials and the treated Ni-Fe-Mo-Co electrode by leaching method, the pre-treated Ni-Fe-Mo-Co electrode has a much lower overpotential and much higher exchange current density for HER. In addition, a long-term continuous electrolysis test with a current interrup- tion shows that the Ni-Fe-Mo-Co alloy has excellent catalytic stability. A new pretreatment method has been developed to improve the catalytic activity of the Ni-Fe-Mo-Co alloy elec trode for hydrogen evolution reaction (HER). The procedure involves pre-electrolzing the Ni-Fe-Mo-Co alloy electrode in 30% KOH solution containing 10% potassium sodium tartrate at 70 ° C for 2 h, until some of the Mo and Fe elements are leached out. The surface morphology of the Ni-Fe-Mo-Co alloy demonstrates a unique hive-like structure after the pre-treatment, which has the pore size in a nanometer range (about 50 nm), a very large real surface area, and good stability. The results of the electrochemical studies show that compared to other similar electrode materials and the treated Ni -Fe-Mo-Co electrode by leaching method, the pre-treated Ni-Fe-Mo-Co electrode has a much lower overpotential and much higher exchange current density for HER. In addition, a long-term continuous electrolysis test with a current interrup- tion shows that the Ni-Fe-Mo-Co alloy has excellent cata lytic stability.