Owing to highly porous and low density attributes, aerogels have been actively utilized in catalysis and adsorption processes, but their great potential in filtration requires exploitation. In this study, an asymmetric aerogel membrane is fabricated via one-pot hydrothermal reaction-induced self-cross-linking of poly(vinyl alcohol) (PVA), which exhibits ultrafast permeation for the separation of oil-in-water emulsion. Meanwhile, carbon nanotubes are added to improve the mechanical strength of the aerogel membranes. The self-cross-linking of PVA forms the supporting layer, and the exchange of water and vapor at the interface of PVA solution and air generates the separating layer as well as abundant hydroxyl groups on the membrane surface. The density, porosity, pore size, and wettability of the aerogel membrane can be tuned by the PVA concentration. Owing to high porosity (>95%) and suitable pore size (<85 nm), the aerogel membrane exhibits high rejection (99.0%) for surfactant-stabilized oil-in-water emulsion with an ultrahigh permeation flux of 135.5 × 103 L m-2 h-1 bar-1 under gravity-driven flow, which is 2 orders of magnitude higher than commercial filtration membranes with similar rejection. Meanwhile, the aerogel membrane exhibits superhydrophilicity, superoleophobicity underwater, and excellent antifouling properties for various surfactant-stabilized oil-in-water emulsions, as indicated by the fact that the flux recovery ratio maintains more than 93% after five cycles of the filtration experiment. The findings in this study may offer a novel idea to fabricate high-throughput filtration membranes.