Spherical-type zirconia granules are successfully fabricated by a spray-drying process using a water solvent slurry, and the change in the green density of the granule powder compacts is examined according to the organic polymers used. Two organic binders, polyvinyl alcohol (PVA) and 2-hydroxyethyl methacrylate (HEMA), which are dissolved in a water solvent and have different degrees of polymerization, are applied to the slurry with a plasticizer (polyethylene glycol). The granules employing a binder with a higher degree of polymerization (PVA) are not broken under a uniaxial press; consequently, they exhibit a poor green density of 2.4 g/cm³. In contrast, the granule powder compacts employing a binder with a lower degree of polymerization (HEMA) show a higher density of 2.6 g/cm³ with an increase in plasticizer content. The packing behavior of the granule powders for each organic polymer system is studied by examining the microstructure of the fracture surface at different applied pressures.