In this work, Cellulose nanofibrils (CNFs) were exposed to the same levels of potassium chloride (KCl) and sodium chloride (NaCl) before being subjected to spray drying. The effect of NaCl and KCl on the size of atomized droplets and the hydrogen bond retardation between CNFs was investigated by characterizing product morphology, particle size distribution, dispersion stability in aqueous system, and surface chemistry. The results showed that the CNF suspensions treated with KCl could be atomized into smaller droplets during spray drying, and then CNF powder with smaller size could be obtained. The agglomeration of CNF was weaker, and the CNF had good dispersion stability after redispersion compared to treat with NaCl. Therefore, KCl treatment before spray drying was an effective method to reduce the agglomeration of CNF during spray drying.