Pickering emulsions play a significant role in generating advanced materials and have widespread application in personal care products, consumer goods, crude oil refining, energy management, etc. Herein, we report a class of wettability tuned silica-based Pickering emulsifiers which stabilize a diverse range of fluid–fluid interfaces: oil/water, ionic liquid/oil, and oil/oil, and their use to prepare microcapsules via interfacial polymerization. To alter particle wettability, colloidal suspensions of SiO₂ particles (22 nm) were modified via silanization with reagents of varied hydrophilicity/hydrophobicity, giving particles that could be dispersed in solvents that became the continuous phase of the emulsions. To test the viability of this system as templates for the fabrication of composite materials, the different particle-stabilized emulsions were coupled with interfacial polymerization, leading to microcapsules with polyurea/silica shells. These results demonstrate that a single particle feedstock can be coupled with fundamental chemical transformation to access a versatile toolkit for the stabilization of diverse fluid interfaces and serve as a template for the preparation of hybrid architectures.