In this study, we explore the impact of monovalent (NaCl) and divalent (CaCl 2 ) brines, coupled with sodium dodecyl sulfate (SDS) surfactant at varying low concentrations, on the detachment and displacement of oil from sandstone rock surfaces. Employing the sessile drop method and molecular dynamics simulations, we scrutinize the behavior of the brine solutions. Our findings reveal that both low salinity and low-salinity surfactant solutions induce a gradual shift in rock wettability toward a more water-wet state. This wettability transformation is not instantaneous but evolves over time, as observed through meticulous molecular motion analyses. Through contact angle measurements and molecular dynamics simulations, we delve into the molecular motion at subpore and micropore scales on sandstone/quartz surfaces. The adsorption of surface-active agents from the oil to the oil−brine interface results in a reduced interfacial tension, significantly contributing to oil displacement. Notably, low salinity concentrations ranging from 1000 to 10,000 ppm exhibit the lowest contact angles within 30 min across all solutions. However, higher concentrations deviate from this declining trend, especially with divalent ions like Ca 2+ , which bridge polar molecules onto the rock surface, resulting in an increased oil-wetting state. This research unveils the intricate molecular motions involved in employing low-salinity surfactant solutions for oil detachment from surfaces. Furthermore, it provides valuable insights into the underlying forces driving oil detachment and wettability alteration.