Stability and rheology of aqueous α-Al2O3 suspensions with poly(methacrylic acid) and poly(acrylic acid) polyelectrolytes were studied as a function of pH, solids loading, and molecular weight. Past work has found polyelectrolyte-stabilized suspensions to be fairly pH independent at low (e.g., 20 vol%) solids loadings. However, we now show that the effective pH range to provide dispersed and fluid suspensions narrows as the concentration of solids increases as related to interparticle forces. At high solids levels, the presence of excess polymer in solution has detrimental effects on stability, which increases as the molecular weight increases. Finally, with knowledge of these concepts, highly concentrated fluid suspensions of 60 vol% Al2O3 (>85 wt%) with submicrometer-size particles have been processed. Higher consolidated densities and reduced sintering temperatures are attained when compared with more conventional processing techniques.