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Oil pollution is caused by the frequent discharge of contaminated industrial wastewater and accidental oil spills and is a severe environmental and health concern. Therefore, efficient materials and processes for effective oil–water separation are being developed. Herein, SiO₂-Na₂SiO₃-coated stainless steel fibers (SSF) with underwater superoleophobic and low-adhesion properties were successfully prepared via a one-step hydrothermal process. The modified surfaces were characterized with scanning electron microscopy (SEM), and contact angle measurements to observe the surface morphology, confirm the successful incorporation of SiO₂, and evaluate the wettability, as well as with X-ray diffraction (XRD). The results revealed that SiO₂ nanoparticles were successfully grown on the stainless-steel fiber surface through the facile hydrothermal synthesis, and the formation of sodium silicate was detected with XRD. The SiO₂-Na₂SiO₃-coated SSF surface exhibited superior underwater superoleophobic properties (153–162°), super-hydrophilicity and high separation efficiency for dichloromethane–water, n-hexane–water, tetrachloromethane–water, paroline–water, and hexadecane–water mixtures. In addition, the as-prepared SiO₂-Na₂SiO₃-coated SSF demonstrated superior wear resistance, long-term stability, and re-usability. We suggest that the improved durability may be due to the presence of sodium silicate that enhanced the membrane strength. The SiO₂-Na₂SiO₃-coated SSF also exhibited desirable corrosion resistance in salty and acidic environments; however, further optimization is needed for their use in basic media. The current study presents a novel approach to fabricate high-performance oil–water separation membranes.