The study uses two numerical models for two-phase liquid simulation-arbitrary Lagrangian-Eulerian method (also referred to as the moving mesh) and the phase-field one-and thorough experimental investigation of the electrodeformation phenomena both in transient and steady-state regimes. Several drawbacks of multiphase electrohydrodynamic process computing are reproduced and explained. Both techniques are applied to the simulation of electrical deformation and coalescence with the quantitative comparison of the results between models as well as with the experiment. The issue of getting unjustified computation results on electrohydrodynamic processes in two-phase immiscible liquids does exist. The experimental quantitative verification of numerical models is of very high complicatedness due to numerous factors that can distort the results. However, the model substantiation can be provided basing on the matching two independent numerical techniques in the range of conditions when both approaches are applicable.