An easy method for green and low-temperature (40°C) reduction of graphene oxide (GO) by increasing the antioxidant activity of green tea polyphenols (GTPs) in the presence of iron was developed. The reduction level (obtained by X-ray photoelectron spectroscopy) and electrical conductivity (obtained by current–voltage measurement) of the GO sheets reduced by GTPs in the presence of iron were comparable to those of hydrazine-reduced GO and much better than those of the GO reduced by only GTPs (in the absence of iron) at reduction temperatures of 40–80°C. Raman spectroscopy indicated that application of GTPs in the presence of iron, in contrast to hydrazine, resulted in better recovering of the sp²-hybridized structure of the sheets. The lasting water dispersion of the polyphenolic-reduced GO sheets in the presence of iron was assigned to π–π adsorption of Fe²⁺-polyphenol radicals on surface of the reduced sheets. A mechanism describing the role of iron in the reduction of the GO by epicatechin gallate and epigallocatechin gallate of green tea was also proposed.