Here, we match the experimental work of adhesion by incorporating surface hydroxylation and water nanolayers of varying thickness at the hematite/PAO4 interface. For the weak (ClayFF 14 ) interaction potential, the simulated work of adhesion aligned with the experimental value with full surface hydroxylation and across all tested water film thicknesses (0-4 ML). For intermediate (INTERFACE-FF ) solid-liquid interactions, good agreement with the experimental work of adhesion occurred with hydroxylated surfaces featuring water films ≥ 1.0 ML, while for strong (Savio et al. ) interactions, the match was observed with water films ≥ 3.0 ML. Previous experiments have suggested that water coverages of ≥ 3.0 ML only form at very high relative humidities (>85%), 22 while water films < 1.0 ML require low relative humidities (<10%). Although the relative humidity conditions for the experimentals used to calculate the work of adhesion are unspecified, it is likely that the steel surface in the experiments had a water film in the 1.0-1.5 ML range. Thus, the strong (Savio et al. ) interaction potential overestimates the adhesive forces between hematite and PAO.