Dyeing of silk with tea polyphenols had natural colors, no toxicity on human security and biodegradable waste with strong social effects and ecological benefits. In this paper, silk was dyed with tea polyphenols and the adsorption isotherm of tea polyphenols in the silk fibers was measured. The analysis showed that adsorption isotherm of tea polyphenols in silk was consistent with Freundlich adsorption model and was also in line with the Langmuir Nernst compound adsorption. Mechanism of action of tea polyphenols and silk was van der Waals force, hydrogen bond and the positioning adsorption of some strong adsorption forces.