Dissipative particle dynamics (DPD) simulations has been performed to study the phase transition of a mixture of cationic and anionic surfactants in an aqueous solution as a function of the total concentration in water and the relative ratio of surfactants. The impact of the relative difference between the tail lengths of the cationic and anionic surfactants on the phase diagram has been simulated by tuning the number of DPD beads in the simulation model. This research also discusses the impact of the frequently used values of the parameters associated with the harmonic bonds among the bonded DPD beads on the obtained self-Assemblies. We find remarkable differences in the resultant self-Assemblies based on different choices of harmonic bond parameters. The performed simulations show an enhanced spectrum of self-Assemblies with augmented tail lengths and disparate harmonic bond parameters. The obtained self-Assemblies are quite unique and can potentially be used in the future for various applications. We also compare the simulation results of the vesicle structures obtained by modeling the electrostatic interaction in the simulation among the charged beads by explicitly introducing charges with a long-range interaction with those obtained by tuning the implicit electrostatic interaction without the long-range interaction. The effects of the chain length of the model and the harmonic bond parameters on the internal density of DPD beads and stress profiles within the vesicles are examined closely. These results are a significant contribution to understanding the stability of the phases and tailoring of the desired vesicles. © 2022 American Chemical Society. All rights reserved.