The exposure of active edge sites of transition metal dichalcogenide (TMD) in TMD-based heterostructures is essential to enhance the catalytic activity toward electrochemical catalytic hydrogen evolution (HER). The construction of TMD-based edge-epitaxial heterostructures can maximally expose the active edge sites. However, owing to the 2D crystal structures, it remains a great challenge to vertically align layered TMDs on non-layered metal chalcogenides. Herein, the synthesis of Cu