Alkali-swellable thickeners (ASTs) such as Acusol 820 and Acusol 830, as well as poly(acrylic acid) homopolymers of various molar mass, have been used as additives in aqueous electrostatically stabilized alumina suspensions. These suspensions have been destabilized by internal enzyme-catalyzed reactions (a direct coagulation casting process) to form viscoelastic solids. The ASTs increase the strength and modulus of the wet green bodies on coagulation. The effect of their molecular architecture on the mechanical properties of wet particulate networks has been studied. At low pH (pH 4.5), ASTs are small insoluble polymer particles that have only minor influence on the low viscosity of the high-solids-loading suspensions. After shifting the pH toward the isoelectric point of α-Al2O3, the suspension coagulates and the AST polymer particles swell, thereby increasing the compressive strength and modulus of the alumina-particulate wet green bodies. The presence of small amounts of ASTs (0.4 wt%, based on the solids loading) results in a 10-fold increase in the strength of the wet green bodies. The compressive strength of the wet green bodies that contain ASTs correlates with the size of the expanded AST molecules at pH 9. A possible explanation is that swelling of the AST particles locally decreases the interparticle distance, which leads to increased van der Waals forces between the ceramic particles.