Molybdenum carbide (Mo2C) is a promising electrocatalyst for hydrogen evolution reaction (HER) due to the similar electron orbital structure to platinum. Preparing Mo2C catalyst in nanoscale increases the exposure of active catalyst site and significantly enhances electrochemical reaction and improve HER performance. However, Mo2C is not a good electron conductor which still requires a more sufficient contact between the catalyst and electrode to transfer electron current. Here, we proposed in-situ Mo2C growth on carbon nanotubes (CNTs) by using wet impregnation of ammonium molybdate tetrahydrate as Mo source, which established a crystalline transition contact between Mo2C and CNTs and significantly improved HER performance. Our results further showed the optimized HER performance of Mo2[email protected]amt and achieved a lower Tafel slopes and low onset potential (ηonset) of 46.7 mV dec−1, 51.3 mV dec−1 and 73 mV and 127 mV (vs. RHE) under alkaline and acidic condition, respectively. Furthermore, Mo2[email protected]amt also shows less attenuation after 1000 times of cyclic voltammograms (CV) cycling stability test and 25 h continuous operation under alkaline and acidic condition.