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Interfacial engineering has been increasingly used to stabilize Pickering emulsions in commercial products and biomedical applications. Pickering emulsion stabilization is aided by interfacial viscoelasticity; however, typically the primary means of stabilization are steric hindrances between high surface concentration shells of particles around the drops. In this work, the concept of creating large interfacial viscoelastic yield stresses with low particle surface concentrations (<50%) using bidisperse charged particle systems is tested to evaluate their potential efficacy in emulsion stabilization. To explore this hypothesis, interfacial rheology and visualization experiments are conducted at o/w interfaces using positively charged amidine, negatively charged carboxylate, and negatively charged sulfate-coated latex spheres and compared to a model based on interparticle forces. Bidisperse particle systems have been observed to create more networked structures than monodisperse systems. For surface concentrations of <50%, bidisperse interfaces created measurable viscoelastic moduli ∼1 order of magnitude larger than monodisperse interfaces. Furthermore, these interfaces have measurable yield stresses on the order of 10–4 Pa·m when monodisperse systems have none. Bidispersity impacts surface viscoelasticity primarily by increasing the overall magnitude of attraction between particles at the interface and not due to changes in the microstructure. The developed model predicts the relative surface fraction that creates the largest moduli and shows good agreement with the experimental data. The results demonstrate the ability to create large viscoelastic moduli for small surface fractions of particles, which may enable stabilization using fewer particles in future applications.