Surface coating is essential and critical to endow fiber materials with various functions for broad applications. However, it is still a great challenge to achieve a fast, fully covered, and robust surface coating on multiple fibers. In this work, a nanoscale surface coating with superior stability was rapidly and integrally formed on various fiber materials (such as Nylon mesh, nonwoven fabrics, and stainless-steel mesh) by highly reactive interfacial polymerization (IP) between polyethylenimine (PEI) and trimesoyl chloride (TMC). The resulting polyamide (PA) layer with an ultrathin thickness of tens of nanometers wholly and uniformly covered the surface of each fiber of the constituent material. Due to the synergistic effect of the PA layer with inherent robustness and the fully covered structure between the outer PA layer and the inner fiber, the nanosurface-coating exhibited outstanding mechanical stability, good acid resistance, and excellent organic solvent resistance. The functional modification of the nanosurface-coating can be easily carried out by using the abundant carboxyl groups in the PA layer. By introducing sulfobetaine zwitterionic copolymers via either "grafting from" or "grafting to" methods, the surfaces presented prominent underwater antioil-adhesion property and exceptional protein adhesion resistance. The surface coating based on IP process opens up an avenue in the field of surface modification. It is expected to offer a generally feasible strategy for the fabrication of fiber materials with robust and multifunctional coatings.