To investigate the effect of the surface properties of dispersed particles on the shear thickening behavior of their corresponding suspensions and further control this characteristic, three kinds of suspensions were prepared by mixing SiO 2 , SiO 2 -NH 2 , and SiO 2 -COOH microspheres with a poly(ethylene glycol) fluid medium, and their rheological behavior was analyzed carefully. Compared to the SiO 2 microsphere suspension, the SiO 2 -NH 2 and SiO 2 -COOH microsphere suspensions show a weaker thickening behavior and a greater critical shear rate due to the aggregation tendency caused primarily by the organic chains. Moreover, the rheological behavior of the three suspensions display different dependencies on the pH value, which is comprehensively determined by the interaction between the microspheres and the medium. Moreover, the critical shear stress of suspensions with different pH values could be predicted by the Wagner model, which basically proves that the interaction between the particles significantly influences the beginning of thickening. The thickening degree could be interpreted by friction theory. The critical volume fraction corresponding to the onset of discontinuous shear thickening is determined by the friction coefficient between the particles, which is greatly affected by the pH value. Investigation of the effect of the surface properties of dispersed particles on the shear thickening behavior of their corresponding suspensions.