The invention presents a preparation method of organic silicone elastomers cross-linked bypolyphenols, which comprises steps as follows: (1) Dissolve 15-250 parts (by mass) of amino-polysiloxanes in the organic solvents to get the amino-polysiloxanes solution; then, dissolve 1˜20 parts of polyphenols in 1-60 parts of water to get the aqueous solution of polyphenols; mix the said two solutions, add 2-130 parts of reinforcement fillers, stir evenly, and then pour them into the mold. (2) Cure and cross-link the mold containing the mixed solutions at 80° C.-170° C. for a period of time, and cool it to room temperature to get the organic silicone elastomer.