Effective ammonia (NH3) adsorbent is crucial for removing undecomposed NH3 residue after splitting into N2 and H2 fuel. In this study, a zeolite-activated carbon (AC) hybrid was successfully synthesized with a trace AC amount and different Si/Al ratios via hydrothermal method. The NH3 adsorption–desorption properties and mechanisms were investigated through two major activity tests, employing high pressure adsorption isotherm analyzer and breakthrough set up. Incorporating AC at 1 wt%, effectively shortened the regeneration period of the pure zeolite by ∼50% due to the AC’s pore-widening effect on zeolite network, reducing the trapping of adsorbed NH3 in the zeolite pores. Interestingly, an optimum Si/Al ratio of 1.6 led to the highest specific surface area of 977.57 m2/g by the formation of zeolite mixture with coexisting NaX (faujasite zeolite with high Al atoms per cell) and NaY (higher crystalline faujasite zeolite with low Al atoms per cell). These improved structural characteristics consequently exhibited the highest NH3 (99.9995 %) storage capacity of 15.6 mmol/g at a partial pressure of 300 kPa in isotherm analysis at 25 °C. Besides, the initial breakthrough adsorption capacity for dilute NH3 (5 %/N2 balance) under atmospheric conditions reached 8.9 mmol/g, accurately equivalent to isotherm analysis result at 5 kPa. This reproducibility of consistent adsorption uptake within low pressure region in both tests was credited to the compositional presence of both acidic and alkaline surface functionalities in the optimum zeolite-AC hybrid as stable NH3 adsorption sites. These active sites also provided a uniform dynamic adsorption capacity of ∼4 mmol/g throughout 15 cycles. Conclusively, this work highlighted the importance of zeolite composition and AC-incorporated proportion for the H2 purification aspect.