With tunable pore size and rich active metal centers, metal-organic frameworks (MOFs) have been regarded as the one of the promising materials for catalysis. Prospectively, employing MOFs in electrochemistry would notably broaden the scope of electrocatalysis. However, this application is largely hindered by MOFs' conventionally poor electrical conductivity. Integrating MOFs without compromising their crystalline superiority holds a grand challenge to unveil their pristine electrocatalytic properties. In this work, we introduce an epitaxial growth strategy to accomplish the efficient integration of the insulating MOFs into electrochemistry. Particularly, with pristine-graphene-templated growth, the two-dimensional (2D) single-crystal MOF possesses a large lateral size of similar to 23 mu m and high aspect ratio up to, similar to 1500 and exhibits a significant electrochemical enhancement, with a charge transfer resistance of similar to 200 ohm and a 30 mA cm(-2) current density at only 0.53 V versus a reversible hydrogen electrode. The epitaxial strategy could be further applied to other 2D substrates, such as MoS2. This MOF/graphene 2D architecture sheds light on integrating insulating MOFs into electrochemical applications.