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Although various superhydrophobic/superoleophilic porous materials have been developed and successfully applied to separate water-in-oil emulsions through the size-sieving mechanism, the separation performance is restricted by their nanoscale pore size severely. In this study, the wettability of underoil water on fumed silica was experimentally observed, and the underlying mechanism was investigated by carrying out theoretical analysis and molecular dynamic (MD) simulations. Further, we present a novel, facile, and an inexpensive technique to fabricate an underoil superhydrophilic metal felt with microscale pores for the separation of water-in-oil emulsions using SiO₂ nanoparticles (NPs) as building blocks. The as-prepared underoil superhydrophilic coating is closed-packed and ultrathin (the thickness is approximately hundreds of nanometers), as well as capable of being coated on a metal felt with …