Here, nitrogen doped molybdenum disulfide quantum dots (N-MoS2 QDs) are fabricated by making use of the pulsed laser ablation (PLA) process in liquid nitrogen (LN2) as a dopant agent. In fact, LN2 contributes the rapid condensation of the plasma plume to form MoS2 QDs, optimizing the conditions for the synthesis of N-doped MoS2 with p-type property. The structural/optical features of the synthesized products are studied using transmission electron microscopy (TEM), absorption spectroscopy, photoluminescence (PL) spectroscopy techniques, and X-ray photoelectron spectroscopy (XPS). The TEM image shows the creation of MoS2 QDs with 5.5 nm average size. UV-vis and PL spectroscopy confirm the formation of N-MoS2 QDs according to the dominant peaks. The Tuck plot gives a direct band-gap of 4.34 eV for MoS2 QDs. Furthermore, XPS spectroscopy reveals Mo-N bonding, indicating nitrogen doping as evidence of p-type MoS2 QDs. Thus, PLA provides a single-stage way to the clean and green synthesis of the MoS2 QDs suspension without a need for high vacuum devices and additional chemical components. Regarding the pristine MoS2, the N-MoS2 QDs benefit from a low overpotential of −0.35 V at −10 mA/cm2 per µg alongside a low Tafel slope of 300 mV/dec. Subsequently, the lower Rct value of N-MoS2 QDs verifies the enhancement of the charge transfer kinetics mainly due to the elevated electronic conductivity. Furthermore, the quasi-rectangular cyclic voltammetry (CV) as well as the larger current window demonstrate a notable electrocatalytic activity. The former is based on the enhanced active sites in favor of N-MoS2 QDs against other samples of interest. Thereby, it is discovered that the N-doped MoS2 QD acts as an effective catalyst to notably improve the performance of the hydrogen evolution reaction (HER).