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Recently, the crude oil spill has brought inevitable harm to the global ecological environment. Due to the high-viscosity crude oil, it is wise to take advantage of the photothermal/electrothermal effects of the membrane to separate the crude oil from the water. However, the functional separation membrane always suffers from low photothermal/electrothermal effects and poor stability. Herein, the vinyl polyvinylidene fluoride/mercapto carbon nanotubes@vinyl-terminated polydimethylsiloxane (PVDF-a/CNT-s@PDMS) membrane with fast photothermal/electrothermal effects and organic absorption property was successfully prepared by electrospinning and multi-layer loading method. The prepared PVDF-a/CNT-s@PDMS membrane resisted a variety of liquids and had stable superhydrophobicity (WCA = 156°). Furthermore, the membrane maintained superhydrophobicity even suffer from water and milk under the applied voltage condition. After 100 wear resistance tests, the membrane maintained stable superhydrophobicity and the separation rate remained unchanged. The surface temperature of the membrane rapidly approached to the maximum temperature in 30 s, showing a rapid photothermal/electrothermal effects, and the average separation rate of crude oil was 1185 kg m−2 h−1·bar−1. Meanwhile, the membrane exhibited outstanding efficiency for separate immiscible oil-water mixtures. Importantly, the incorporation of the sulfhydryl group enhanced the special ability of the composite membrane to adsorb organic dyes from oil phase. Therefore, the PVDF-a/CNT-s@PDMS membrane has a wide range of potential application in the domain of oil-water separation. [Display omitted] • The superhydrophobic membrane exhibited high stability toward abrasion. • The obtained membrane possessed fast photothermal/electrothermal response. • The membrane effectively achieved various oil/water mixture separation. • The membrane possessed ability for the adsorption of organic dyes from the oil phase. [ABSTRACT FROM AUTHOR]