The uniform coating of catalytic materials on the electrode surface is essential for improving the performance of electrochemical reactions. In this study, the electrostatic spray coating technique is used to deposit Molybdenum disulfide (MoS2) particles on carbon electrodes and examine the electrochemical hydrogen evolution reaction (HER) performance in a 0.1 M H2SO4 electrolyte. The experimental results reveal that the electrostatic spray coating method achieves a more uniform coating MoS2 catalyst particles on the carbon fiber substrate. It provides good adhesion for electrocatalyst binding on the carbon paper electrodes. During HER analysis, a 25% higher current density is obtained from the electrostatic spray-coated electrodes compared to the manual spray-coated electrode at a potential of 0.95 V. Electrochemical impedance spectroscopy, and electrochemical surface area measurements indicate the superior electrochemical characteristics of the electrostatic spray-coated electrode. The faradaic efficiency of the electrostatic spray-coated electrode is close to 100% at a high applied potential of −1.6 V with a 0.0059 L volume of hydrogen generation. Moreover, chronoamperometric measurements demonstrate the excellent durability of the electrostatic spray-coated carbon electrodes. This study suggests that the facile electrostatic spray method is efficient for coating electrodes with high uniformity and good adhesion for various electrochemical applications.