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The non-selective property of conventional polyurethane (PU) foam tends to lower its oil absorption efficiency. To address this issue, we modified the surface properties of PU foam using a rapid solvent-free surface functionalization approach based on the chemical vapor deposition (CVD) method to establish an extremely thin yet uniform coating layer to improve foam performance. The PU foam was respectively functionalized using different monomers, i.e., perfluorodecyl acrylate (PFDA), 2,2,3,4,4,4-hexafluorobutyl acrylate (HFBA), and hexamethyldisiloxane (HMDSO), and the effect of deposition times (1, 5 and 10 min) on the properties of foam was investigated. The results showed that all the modified foams demonstrated a much higher water contact angle (i.e., greater hydrophobicity) and greater absorption capacities compared to the control PU foam. This is due to the presence of specific functional groups, e.g., fluorine (F) and silane (Si) in the modified PU foams. Of all, the PU/PHFBAi foam exhibited the highest absorption capacities, recording 66.68, 58.15, 53.70, and 58.38 g/g for chloroform, acetone, cyclohexane, and edible oil, respectively. These values were 39.19–119.31% higher than that of control foam. The promising performance of the PU/PHFBAi foam is due to the improved surface hydrophobicity attributed to the original perfluoroalkyl moieties of the HFBA monomer. The PU/PHFBAi foam also demonstrated a much more stable absorption performance compared to the control foam when both samples were reused for up to 10 cycles. This clearly indicates the positive impact of the proposed functionalization method in improving PU properties for oil absorption processes. [ABSTRACT FROM AUTHOR]