Water-based nanofluids were successfully prepared using stably dispersed graphene oxide (GO) and MgO nanoparticles (NPs), and applied to cold rolling lubrication. The findings of the study demonstrate that the incorporation of GO/MgO nanofluid leads to a substantial reduction in rolling force, minimum rolling thickness (0.314 mm), and surface roughness (0.348 μm). This enhancement is ascribed to the presence of a bilayer in-situ friction film, with a thickness of approximately 50 nm. This film consists of a chemically reaction layer (consisting of Fe 2O 3, FeO, and Mg(OH) 2) and a physically adsorbed layer (primarily NPs fragments). Molecular dynamics simulations revealed a combination of synergistic effects between GO and MgO, achieving anti-wear and friction reduction through multiple mechanisms, including interlayer sliding, rolling, filling, and polishing. The calculations demonstrated that, in comparison with GO or MgO simulation systems alone, the percentage of MgO rolling motion in the GO/MgO system increased from 72% to 82%, while the transferred friction force percentage increased from 3.8% to 14.2%.