Direct casting is a processing method that can produce large parts of complex geometry. It uses dispersions of ceramic particles in water and a hydraulic binder for consolidation. Studies on castable structures have reported the generation of a significant fraction of pores due to the presence of water. This effect occurs because drying preserves part of the interparticle pores originally occupied by water. The fraction of pores obtained in these cases can reach levels higher than 50%, affecting the properties of the structure. However, the porogenic behavior of water in these materials was not investigated in depth. In this work, aqueous suspensions of calcined alumina and hydratable alumina (hydraulic binder) of different water contents (40–60 vol.%) were prepared in a paddler mixer. For compositions of lower (5–35 vol.%) or higher (66–80 vol.%) water amounts, casting and curing steps were assisted by external pressure and a rotating device, respectively, to produce homogeneous microstructures. The total porosity after drying was similar to the initial volumetric content of water in the compositions when side effects, such as sedimentation and air entrapment, were prevented. Below water content of 25 vol.%, particles packing flaws became the main pore generator and the hydroxylation reaction of the binder no longer occurred effectively.