In general, block crystals tend to cake and have poor flowability. Changing the crystal shape to sphericity is useful to overcome those disadvantages. In this work, spherical agglomerates of potassium borohydride (KBH 4 ) were prepared by the antisolvent crystallization method (ACM) with the assistance of KOH. Two different antisolvents tetrahydrofuran (THF) and acetonitrile (ACN) were selected and compared. Both spherical agglomerate products have improved flowability and anticaking ability compared with commercial KBH 4 . Moreover, based on in situ observation, it was proposed that both spherical crystallization processes followed two agglomeration stages, but KBH 4 experienced different primary agglomeration in two antisolvents. The compact crystallization in droplets makes the spherical agglomerates prepared in THF more spherical and denser than those prepared in ACN. It was found that KOH significantly promoted the secondary agglomeration, therefore resulting in large spherical agglomerates. The size of the spherical agglomerates can be tuned from hundreds of micrometers to several millimeters by changing process parameters in the presence of KOH. The comparison study in this work shows a great relationship between mechanisms and properties of KBH 4 spherical agglomerates, and it provides guidelines for the design of other spherical agglomerates.