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A new concept of enzymatic coloration of silk fiber with tea polyphenols (TP) in the presence of Rhus vernicifera Laccase was proposed in this study. Three methods were investigated: the simultaneous enzymatic polymerization of TP and coloration of silk, the polymerization of TP with laccase followed by a further coloration of silk, and the adsorption of TP by silk followed by laccase treatment. All the methods, especially the first two methods can increase the color depth of silk and improve the color fastness. The color depth of silk increases with the dyeing time and the laccase concentration up to 4 U/mL at pH 5.0 and 50oC.