Calcium chloride (CaCl2) impregnated zeolite A and strontium chloride (SrCl2) impregnated zeolite A and X composite granules were evaluated as ammonia sorbents for automotive selective catalytic reduction systems. The SrCl2-impregnated zeolite A granules showed a 14% increase in ammonia uptake capacity (8.39 mmol g−1) compared to zeolite A granules (7.38 mmol g−1). Furthermore, composite granules showed 243% faster kinetics of ammonia sorption (0.24 mmol g−1 min−1) compared to SrCl2 (0.07 mmol g−1 min−1) in the first 20 min. The composite CaCl2/SrCl2 impregnated zeolite A granules combined the advantages of the zeolites and CaCl2/SrCl2, where the rapid physisorption from zeolites can reduce the ammonia loading and release time, and chemisorption from the CaCl2/SrCl2 offers abundant ammonia capacity. Moreover, by optimizing the content of SrCl2 loading, the composite granules maintained the granular form with a crushing load of 17 N per granule after ammonia sorption–desorption cycles. Such structurally stable composite sorbents offer an opportunity for fast ammonia loading/release in automotive selective catalytic reduction systems.