A novel agglomerated crystallization technique, termed spherical crystallization technique, which can transform fine crystals precipitated into spherical agglomerates in one step during the crystallization process, has been developed by using new agglomeration phenomena of particles in liquid system. In this technique, a binary or a ternary mixture of partially miscible solvents was used as a crystallization solvent. It was found that by choosing the proper proportion of the mixture, a small amount of immiscible liquid was liberated from the system, which could preferentially wet the crystals, forming spherical agglomerates. By using this technique, needle like crystals of salicylic acid were agglomerated into spheres being directly compressible into tablet. Spherically agglomerated crystals of aminophylline were prepared directly by reacting theophylline with ethylenediamine in an alcohol-organic solvent-water mixture. The spherically agglomerated crystals of new complex of indomethacin and epirizole with increased solubilities were prepared. Controlled release microspheres of ibuprofen with acrylic polymer were prepared to improve bioavailability.