One of the current global challenges is to find renewable, low-carbon, and clean substitutes for fossil fuels. Hydrogen (H 2 ) can be seen as the ideal energy carrier for the future to change the global energy structure. As water is an abundant source, large-scale production of pure hydrogen from water electrolysis using a suitable catalyst seems to be a good alternative to steam reforming. It is therefore very important to search for low-cost, earth-available, and efficient catalysts for the hydrogen evolution reaction (HER). In this work, a novel 2D/2D nanoheterointerface was built between titanium carbo-oxide (TCO) and molybdenum sulfide (MoS 2 ) using an easy and onepot solvothermal method. Characterizations by X-ray diffraction, Raman spectroscopy, scanning electron microscopy, transmission electron microscopy, and X-ray photoelectron spectroscopy demonstrate that the targeted material with increased defects in the heterostructure was successfully obtained. The prepared nanohybrid material exhibits significantly better electrocatalytic properties than pristine TCO and MoS 2 for the HER in an acidic medium. An overpotential of 269 mV (at the current density of 10 mA cm −2 ), a Tafel slope of 82 mV dec −1 , and very high stability with an overpotential loss of only 17.06 mV after 5000 cycles were obtained. The enhancement of HER properties in the nanohybrid material is derived from the increase in defects with the formation of the nanoheterointerface, which activates a new catalytic site in the basal plane of MoS 2 , thus enhancing the electrocatalytic properties.