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Traditional polyamide-based interfacial polymerized nanofiltration (NF) membranes exhibit upper bound features between water permeance and salt selectivity. Breaking the limits of the permeability and rejections of these composite NF membranes are highly desirable for water desalination. Herein, a high-performance NF membrane (TFC-P) was fabricated via interfacial polymerization on the poly(vinyl alcohol) (PVA) interlayered poly(ether sulfone) (PES) ultrafiltration support. Owing to the large surface area, great hydrophilicity, and high porosity of the PES–PVA support, a highly cross-linked polyamide separating layer was formed with a thickness of 9.6 nm, which was almost 90% thinner than that of the control membrane (TFC-C). In addition, the TFC-P possessed lower ζ-potential, smaller pore size, and greater surface area compared to that of the TFC-C, achieving an ultrahigh water permeance of 31.4 L m^–2 …