Developing stable, surfactant-free formulations for food, pharmaceutical, and cosmetic applications remains a challenge due to the high environmental impact and toxicity risks associated with synthetic surfactants. While solid particles offer an eco-friendly alternative for establishing kinetic stability in Pickering emulsions, the performance of natural, unmodified aluminosilicate clays remains highly variable and poorly optimized. This study aimed to solve this limitation by systematically mapping the stabilization performance of raw bentonite and kaolin using targeted mechanical milling and ionic-strength adjustments without relying on chemical surface modifications. The mineral matrices were characterized using X-ray diffraction, Fourier-transform infrared spectroscopy, and electron microscopy to link structural amorphization to interfacial performance. Oil-in-water formulations were prepared via high-shear homogenization by systematically adjusting clay content, oil volume fraction, and phase salinity, utilizing a central composite design and response surface methodology to model system stability. The experimental results demonstrated that mechanical processing yielded optimized particle-size distributions capable of organizing rigid interparticle networks at the oil–water interface. Rheological modeling confirmed solid-sphere behavior and thixotropy under optimal concentrations, proving that physical processing and electrolyte control are sufficient to engineer highly stable, green Pickering systems tailored for targeted industrial applications.