Near net-shaped parts of zircona-alumina composites have been successfully formed by gelcasting, a technique which utilizes in situ polymerization of acrylamide monomers. The high solids loading required for gelcasting (∼S0 vol%) was obtained by controlling the pH-dependent stability of the aqueous zirconia-alumina suspensions. A strong correspondence was found among the surface charges on the particles, colloidal stability, and the maximum solids loading.