Conventional textile dyeing relies on the use of dyes and pigments, which can cause severe environmental contamination and waste a large amount of water. Structural coloring is one of the effective ways to achieve environmentally friendly coloring of textiles. In this work, three plant polyphenols with the same o-benzenetriol structure (tannic acid (TA), gallic acid (GA), and tea polyphenol (TP)) were selected as raw materials. Three plant polyphenols can quickly form nanofilms at the gas-liquid interface through a Schiff base reaction with polyethyleneimine (PEI) under mildly alkaline conditions, which were deposited to the surface of silk fabric, allowing precise control over the thickness of film by adjusting the time, resulting in various structurally colored silk fabric. This method for creating structural colors is not substrate-specific and enables the quick production of structural colors on various textile substrates. Furthermore, the structural color silk fabric based on plant polyphenol has antibacterial performance. This textile coloring method is simple, cost-effective and environmentally friendly, providing a new approach to eco-friendly textile dyeing.