Adsorbed phosphate on smooth platelet α-Al2O3 particles at saturation surface coverage gives rise to strong interparticle attractive forces in dispersion. The maximum yield stress at the point of zero charge was increased by 2-fold. This was attributed to a high density of intermolecular hydrogen bonding between the adsorbed phosphate layers of the interacting particles. Adsorbed citrate at saturation surface coverage, however, reduced the maximum yield stress by 50%. It adsorbed to form a very effective steric barrier as intramolecular hydrogen bonding between −OH and the free terminal carboxylic group prevented strong interactions with other adsorbed citrate molecules residing on the second interacting particle. This steric barrier kept the interacting platelet particles further apart, thereby weakening the van der Waals attraction. The platelet α-Al2O3 dispersions were flocculated at all pH level. These dispersions displayed a maximum yield stress at the point of zero zeta potential at the pH ≈ 8.0. They also obeyed the yield stress-DLVO force model as characterized by a linear decrease in the yield stress with the square of the zeta potential.