Wettability alteration of oil-wet calcite by surfactants was studied by means of molecular dynamics (MD) simulations. The simulations use the recently developed model for positively charged calcite surface, whose oil-wet state originates from binding of negatively charged carboxylate molecules contained in the oil, consistently with the bulk of the available experimental data. The ability to alter the surface wettability, which can be directly quantified by the release of the surface-bound carboxylates, is tested for nine different surfactants of all charge types-cationic, anionic, nonionic, and zwitterionic-and compared to that of brine. It was found that only the cationic surfactants are able to detach the organic carboxylates more efficiently than brine, while the neutral and anionic surfactants do not seem to have any measurable effect on the wettability. The outperformance of the cationic surfactants is generally consistent with the majority of previously published experimental observations. The data also point toward a consistently better performance of single-tailed cationic surfactants over the two-tailed structure. Molecular mechanism of the wettability alteration by different types of surfactants is discussed, along with the implications of the results for the design of new surfactant formulations for the enhanced oil recovery.