Improved oil recovery from asphaltenic oil reservoirs may provide the world with a significant source of lower-cost energy over many decades. However, the mechanisms through which the surface-active components in crude oil, such as asphaltenes and organic acids, affect incremental oil production are still unclear. In this study, we investigate crude oil/water interfacial films using shear and dilational rheology for mechanical properties and Fourier-Transform Infrared Spectroscopy (FTIR) to better understand its molecular species present at the interface that contribute to the development of viscoelastic behaviors. Dilational rheology has proven to be more sensitive to early time development of elasticity. In contrast, shear rheology provided more insights regarding the formation of elastic films at the macroscopic scale and late time interfacial changes. The presence of salts such as sodium chloride in the aqueous phase played a critical role in altering the dynamics of both the rheological properties development and the interfacial tension.