The structural engineering of 2D layered materials is emerging as a powerful strategy to design catalysts for high-performance hydrogen evolution reaction (HER). However, the ultimate test of this technology under typical operating settings lies in the reduced performance and the shortened lifespan of these catalysts. Here, a novel approach is proposed to design efficient and robust HER catalysts through out-of-plane deformation of 2D heterojunction using metal-organic chemical vapor deposition. High-yield, single-crystalline WTe2 nanobelts are used as an epitaxial template for their coherent conversion to WS2. During the conversion process, the WTe2/WS2 heterostructure containing both lateral and vertical junctions are achieved by coherent heteroepitaxial stacking despite differences in symmetry. The lattice coherency drives out-of-plane deformation of heteroepitaxially grown WS2. The increase in the effective surface area and decrease in the electron-transfer resistance across the 2D heterojunctions in turn enhances the HER performance as well as the long-term durability of these electrocatalysts.