Shear thickening fluid (STF) is a smart material that has a certain response when subjected to external shear stress, and has received widespread attention for its unique feature. Herein, we synthesized mesoporous silica and prepared an STF with mesoporous silica as the dispersed phase, and introdued fumed silica to create a novel multi-phase STF. The multi-phase STF containing fumed silica has a lower critical shear rate and a higher peak viscosity. The reason for this is that the unique pore structure of mesoporous silica makes the system easier to disperse. In addition, the addition of fumed silica also fills the pores around the mesoporous silica as much as possible. The occurrence of particle clogging is easier, and the mutual contact between the particles can form a more stable friction contact network. In terms of impact resistance, the impact crater volume decreases significantly with increasing fumed silica additions. In particular, at 17 wt% fumed silica, the impact crater volume is only 3.03 × 10 5 μm, which is a full order of magnitude less than that of the specimen without STF additions. The rheological properties and impact resistance of multi-phase STF based on fumed silica modulation are systematically investigated, and a feasible strategy to modulate the interactions between fluid structures to develop high-performance STFs is introduced.