HypothesisIt is possible to control the absolute and relative magnitude of repulsive and attractive interactions and hence microstructure of interfacial particles at and air/water interface by adjusting subphase composition. It should be possible to modify interfacial viscoelasticity from elastic to viscous behavior through these changes to interfacial microstructure. ExperimentsParticle laden interfaces are made from micron sized polystyrene at an air/water interface. The inter-particle interactions are controlled by the subphase salt concentration and addition of both non-ionic and ionic surfactants. These interfaces are then characterized using an interfacial rheometer with a custom visualization system. FindingsThree distinct microstructures are observed. Low repulsion and high attraction systems exhibit a soft glassy rheology with a disordered but dense microstructure. Creating high repulsion results in a dense hexagonal crystal. Finally, in systems with reduced repulsion and attraction, a hexatic phase can be observed. Each of these microstructures exhibit unique interfacial viscoelastic behavior. These results indicate that control over the properties of these interfaces, and hence Pickering emulsions, is possible through manipulation of interparticle forces.