This paper proposes a comparative study of two techniques of granulation of a submicronic alumina powder with high binder content slurries, by spray drying and freeze granulation for the preparation of mixed granules. First, the viscosity and flow index of the suspensions are given as a function of dispersant, solid and binder contents versus alumina content, and the data are analysed in order to give a predictive model in a wide range. Suspensions with varying viscosities (7–208 mPa.s), densities (1.31–1.76) and surface tensions (23–40 mN/m) were then granulated. The first observations reveal the importance of the content and the molar mass of the binder: when they are too high, the freeze granulation fails and filaments are produced instead of granules due to extensive stretching of the molecular chains of the binder during spraying. Then through a theoretical analysis of the phenomena leading to granulation, an original dimensionless number is proposed to describe the evolution of the granule size as a function of suspension formulation. This number is related to the Reynolds and Weber number and is able to predict the granule size over a wide range (20–500 μm for freeze granulation, and 5–30 μm for spray drying). Spray drying leads to smaller granules with various shapes, from full shape to hollow or donut-like, whereas freeze granulation leads to bigger but spherical granules with a microporosity, and a size easier to predict as no drying shrinkage is observed.