We prepared two kinds of silica. based nanoscale ionic materials( NIMs) with increasing SiO2 con. tents, and also with different relative ionic interaction strengths between their constituents( SiO2-SIT-M2070> SiO2-SIT-Ethomeen for the relative ionic interaction strength). The results of transmission electron microscope ( TEM) and small. angle X-ray scattering( SAXS) investigations indicated that there was no obvious nano. particle aggregate in both kinds of NIMs. The differential scanning calorimetry( DSC) results showed that the ionic interactions prohibited the crystallization of out. shell block copolymers in the prepared NIMs. Moreover, the crystallization suppression was more serious with increasing the ionic interaction strength. Ionic interaction also displayed the dramatic influence on the dynamic rheological behavior of as. prepared NIMs. The dynamic shear moduli and viscosities of SiO2-SIT-Ethomeen were about 1- 3 orders of magnitude lower than those of SiO2-SIT-M2070 with the same solid contents. Under the shear of large dynamic strain, SiO2-SIT-M2070with the relatively high solid contents showed the soft glass rheological properties, while SiO2-SIT. Ethomeen showed the phenomenon of strong strain overshoot. Furthermore, the strain that corresponding with the maximum of dynamic shear moduli and viscosities gradually decreased with the increasing of solid contents, and so did the degree of overshoot. All above results suggested that the rheological properties of NIMs could be effectively controlled by carefully tuning the ionic interactions between their constituents.