Ammonia (NH3), which has a 17.7 wt% gravimetric hydrogen density, has been considered as a potential hydrogen storage material. This study looked at the thermocatalytic decomposition of NH3 using a bulk Mo2N catalyst that was boosted by alkali metals (AM: 5 wt% Li, K, Cs). The K-Mo2N catalyst outperformed all other catalysts in this experiment in terms of catalytic performance. At 6000 h−1 GHSV, 100% conversion of NH3 was accomplished using the K-Mo2N, Cs-Mo2N, and Mo2N catalysts. However, when compared to other catalysts, K-Mo2N had the highest activity, or 80% NH3 conversion, at a lower temperature, or 550 °C. The catalytic activity exhibited the following trend for the rate of hydrogen production per unit surface area: K-Mo2N > Cs-Mo2N > Li-Mo2N > Mo2N. Up to 20 h of testing the K-Mo2N catalyst at 600 °C revealed no considerable deactivation.