Self-standing binder-free materials have been intensively used as electrocatalytic electrodes for hydrogen production. Herein, the binder-free molybdenum selenide nanosheets on threedimensional macroporous reduced graphene oxide/graphite-like membrane (MoSe 2 /rGO-PGM) were proposed. A unique interconnected macroporous conducting carbon membrane was prepared by cryogelation and subsequent carbonization of the gelatin and graphene oxide cryogel. The conducting membrane is used as a substrate to synthesize MoSe 2 by the solvothermal method in which MoSe 2 -layered nanosheets are vertically grown on the surface. The MoSe 2 /rGO-PGM was applied as an electrocatalyst without binder "binder-free" for the water-splitting "hydrogen evolution reaction (HER)". The excellent electrochemical hydrogen generation exhibited a low onset potential of −0.15 V versus the reversible hydrogen electrode and a Tafel slope of 51 mV/decade. In addition, remarkable stability with no current decay for over 20,000 s of testing was observed. The perpendicular oriented nanostructure of the electrocatalyst on a highly carbon-based macroporous template favored more exposed active sites accompanied by an easily diffused electrolyte. The fabrication concept was successfully extended to synthesize other metal dichalcogenides which can be utilized as alternative nanomaterials for HER catalysts.

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