Exploring and designing efficient, cost-effective, and stable non-noble catalysts for the hydrogen evolution reaction (HER) is of critical importance for clean energy applications. Metal-organic frameworks (MOFs) have recently emerged as promising precursors to construct efficient non-noble metal electrocatalysts. Herein, An Assembly of MoMOF/ Zif67/MoMOF as a hybrid of MOF-on-MOF heterostructure has been synthesized. The one dimensional MoMOF was used as precursor to continue the step-by-step synthesis. In order to overwhelm the poor electrical conductivity the synthesized MOF-on-MOF was carbonized. The electrocatalyst with unique design and properties revealed impressively low onset overpotentials of 44 mV and 68 mV at a current density of 10 mA cm−2 towards HER. It also demonstrated a good working stability for the HER in acidic media could be considered as a good alternative of noble metal electrocatalyst. The designed MoMOF/ Zif67/MoMOF showed a satisfactory result of 154 mV overvoltage at a current density of 10 mA cm−2 may be originate from the synthesis strategy and open a new window to direct use of MOF by MOF-on-MOF design.