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The ability to generate hydrogen in an economic and sustainable manner is critical to the realization of a future hydrogen economy. Electrocatalytic water splitting into molecular hydrogen using the hydrogen evolution reaction (HER) provides a viable option for hydrogen generation. Consequently, advanced non-precious metal based electrocatalysts that promote HER and reduce the overpotential are being widely researched. Here, we report on the development of MoS₂-carbon inter-overlapped structures and their applicability for enhancing electrocatalytic HER. These structures were synthesized by a facile hot-injection method using ammonium tetrathiomolybdate ((NH₄)₂MoS₄) as the precursor and oleylamine (OLA) as the solvent, followed by a carbonization step. During the synthesis protocol, OLA not only plays the role of a reacting solvent but also acts as an intercalating agent which enlarges the interlayer spacing of MoS₂ to form OLA-protected monolayer MoS₂. After the carbonization step, the crystallinity improves substantially, and OLA can be completely converted into carbon, thus forming an inter-overlapped superstructure, as characterized in detail using X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy, transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). A Tafel slope of 118 mV/dec is obtained for the monolayer MoS₂-carbon superstructure, which shows a significant improvement, as compared to the 202 mV/dec observed for OLA-protected monolayer MoS₂. The enhanced HER performance is attributed to the improved conductivity along the c-axis due to the presence of carbon and the abundance of active sites due to the interlayer expansion of the monolayer MoS₂ by OLA.