A theory that describes the electroviscoelastic behavior of liquid-liquid interfaces has been developed and applied to an experimental system. A new approach for the analysis of the physical nature of the structure of electrified liquid-liquid interfaces has been proposed. Also, the stability of the secondary liquid-liquid droplet or droplet-film structure in a polydispersed system has been discussed. Three interrelated forms of instability are postulated: rigid, elastic, and plastic. These events are understood as interactions between the internal and external periodical physical fields. The theory is linear to the extent that the rigid form of instability is discussed, but nonlinear when elastic and plastic forms of instabilities take place. A method and apparatus were developed to monitor voltametrically the electrical interfacial potential appearing during the formation of the electrical double layer, while the dropped two phase contact occur. NMR spectroscopy was used for determination of the resonant/characteristic frequency of the molecular complex that builds the secondary liquid-liquid droplet-film structure. The experimental results were in fair agreement with the postulated theory.