AbstractMetal organic framework (MOF)‐based materials have been widely studied and reported as efficient electrocatalysts for the hydrogen evolution reaction (HER), owing to their high surface areas, controllable structures, and tunable pore sizes. However, the intrinsically poor electrical conductivity of most MOFs hinders their directly applications as electrocatalysts. Herein, copper‐centered MOFs (HKUST‐1) have been electrodeposited directly onto the current collector. These electrochemically prepared HKUST‐1@carbon paper hybrids exhibited significantly enhanced electrocatalytic performances for the HER, including a positively shifted of onset potential, a lower overpotential, and a smaller Tafel slope, as compared to the conventional hydrothermally prepared HKUST‐1. The proposed electrodeposited synthesis strategy for MOF‐based electrocatalysts is fast, efficient, mild, and environmentally friendly. This work may also extend to other MOF materials and any conductive substrate, thus providing a facile strategy for the preparation of MOF‐based catalysts with high efficiency and low cost.