The noble, metal-free materials capable of efficiently catalyzing water splitting reactions currently hold a great deal of promise. In this study, we reported the structure and electrochemical performance of new MoS2-based material synthesized with L-cysteine. For this, a facile one-pot hydrothermal process was developed and an array of densely packed nanoplatelet-shaped hybrid species directly on a conductive substrate were obtained. The crucial role of L-cysteine was determined by numerous methods on the structure and composition of the synthesized material and its activity and stability for hydrogen evolution reaction (HER) from the acidic water. A low Tafel slope of 32.6 mV dec−1, close to a Pt cathode, was registered for the first time. The unique HER performance at the surface of this hybrid material in comparison with recently reported MoS2-based electrocatalysts was attributed to the formation of more defective 1T, 2H-MoS2/MoOx, C nanostructures with the dominant 1T-MoS2 phase and thermally degraded cysteine residues entrapped. Numerous stacks of metallic (1T-MoS2 and MoO2) and semiconducting (2H-MoS2 and MoO3) fragments relayed the formation of highly active layered nanosheets possessing a low hydrogen adsorption free energy and much greater durability, whereas intercalated cysteine fragments had a low Tafel slope of the HER reaction. X-ray photoelectron spectroscopy, scanning electron microscopy, thermography with mass spectrometry, high-resolution transmission electron microscopy, Raman spectroscopy techniques, and linear sweep voltammetry were applied to verify our findings.