The behavior of mineral mixtures can be significantly different from the behavior of the individual components of the mixture due to differences between the mechanical and chemical properties of the individual minerals, and their ensuing effects on interparticle interactions and fabric formation. This study examines mixtures of kaolinite and calcium carbonate at different mass fractions using sedimentation, viscosity, and liquid-limit tests. These macroscale tests represent a wide range of solid-volume fractions and strain levels, with emphasis on high water-content conditions to magnify the effects of electrical forces. The results demonstrate that interparticle interactions depend on mineral surface-fluid effects, particle geometry, relative particle size, and solids content. With small solids contents, the kaolinite/calcium carbonate mixture behavior is a function of electrostatic interactions between oppositely charged mineral particles that promote flocculation; however, with large solids contents, the specific surface area of the minerals is the controlling factor. These results are relevant to many natural soil environments and to the possible development of engineered mineral mixtures for industrial applications.