Two-dimensional transition metal-dichalcogenides are emerging as efficient and costeffective electrocatalysts for hydrogen evolution reaction (HER). However, only the edge sites of their trigonal prismatic phase show HER-electrocatalytic properties, while the basal plane, which is absent of defective/unsaturated sites, is inactive. Here, we tackle the key challenge that is increasing the number of electrocatalytic sites by designing and engineering heterostructures composed of single-/few-layer MoSe 2 flakes and carbon nanomaterials (graphene or single-wall carbon nanotubes (SWNTs)) produced by solution processing. The electrochemical coupling between the materials that comprise the heterostructure effectively enhances the HER-electrocatalytic activity of the native MoSe 2 flakes. The optimization of the mass loading of MoSe 2 flakes and their electrode assembly via monolithic heterostructure stacking provided a cathodic current density of 10mAcm -2 at overpotential of 100mV, a Tafel slope of 63mVdec -1 and an exchange current density (j 0 ) of 0.203µAcm -2 . In addition, electrode thermal annealing in a hydrogen environment and chemical bathing in nbutyllithium are exploited to texturize the basal planes of the MoSe 2 flakes (through Sevacancies creation) and to achieve in situ semiconducting-to-metallic phase conversion, respectively, thus they activate new HER-electrocatalytic sites. The as-engineered electrodes show a 4.8-fold enhancement of j 0 and a decrease in the Tafel slope to 54mVdec -1 .