The main objective of this investigation is to describe the interaction between cement hydrates and electrolyte solution to understand multi-ionic transport in cementitious materials. A surface complexation model in PHREEQC including an electrostatic term is used to simulate the ionic adsorption on the calcium silicate hydrate (C-S-H) surface. The equilibrium constants for the adsorption of ions on C-S-H surfaces are obtained by fitting experimental data to the model. The adsorption of both divalent and mono-valent cations, and also anions significantly changes the surface charges of hydrated paste. Chloride is being held in a chemical binding as Friedel's salt and bound mainly by the adsorptive action of C-S-H. An integrated modelling approach employing a phaseequilibrium model, a surface complexation model, and a multi-component diffusion model has been developed in PHREEQC to simulate the multi-ionic transport through hydrated cement paste. It was found that the physical adsorption of ions on C-S-H, the size of pores, and the surface site density of C-S-H govern the rate of penetration of ionic species. Finally, the proposed model has been validated against chloride profiles measured in this study as well as with data available in the literature for hydrated cement paste.