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This invention provides a method for synthesizing novel natural pigments using phenotypic catechins. Various epicatechins, epigallocatechins, epicatechin gallate esters, and epigallocatechin gallate esters are used as substrates. These are mixed and subjected to a non-enzymatic oxidation reaction under humid and hot conditions to generate a new class of tea pigment compounds. The non-enzymatic oxidation products of the phenotypic catechins are then concentrated under reduced pressure, freeze-dried, extracted, and purified by column chromatography to obtain dimeric catechin pigments. The six novel dimeric catechin pigments obtained by this invention are synthesized using a simple method. The six novel dimeric catechin pigments obtained according to the method of this invention are orange-yellow or orange-red amorphous powders with good color-adjusting capabilities, and can be applied to coloring tea beverages and new-style tea drinks. The discovery of this type of natural pigment contributes to the research on coloring substances during the thermal processing of tea, the improvement of tea liquor color quality, and the development and application in the field of food coloring.