In this research, two different particle sizes of kaolin were selected, and their rheological properties were characterized by steady-state and dynamic rheological tests. Stress relaxation in the flow curves was a novel finding; redefinition and interpretation of flow curves were the focus of our research. Two methods were used and compared for determining the yield stress. The results showed that suspensions with higher solid content and smaller particle size showed more compact inter-particle interactions, exerting multiple stress relaxation and a strong yield and viscoelastic characteristic. The thixotropic properties were also strongly affected by solid content and particle size, and the differences were reflected in the structural recovery capability. Finally, the effects on rheological properties by introducing deflocculant were studied; the stress relaxation disappeared gradually, and storage modulus and yield stress increased.Moreover, kaolin suspensions with smaller particle sizes required more deflocculant for adsorption and electrical neutralization, confirming that more positively charged edges were exposed after fragmentation. This study has provided an excellent approach to control and adjust the rheological properties of kaolin suspensions in industrial applications.