The purpose of this article is to explore the role of viscoelastic properties of polymeric solutions on the jet mode in the electrospray process. In this research, several numerical simulations were performed to model the behavior of electrified Newtonian and viscoelastic jets. First, used for validating viscoelastic constitutive equations and their implementation, the benchmark problem of the sedimenting sphere is stabilized beyond the previously suggested threshold. Then, an electrified DI water jet was simulated, and the obtained jet profile was compared with the experimental data from previous publications. Finally, the proposed algorithm was used to simulate viscoelastic electrified jets, where the effect of the Weissenberg number (Wi) on the jet profile was examined. In agreement with the previously obtained experimental results, by increasing the solution concentration, the asymptotic profile of the jet is reached at a smaller length from the nozzle, while the final thickness of the jet is slightly reduced.