The invention relates to the organic second-order nonlinear optical material field, and especially relates to an organic second-order nonlinear optical chromophore having a D-pi-A structure, and a synthetic method and a use thereof, wherein the organic second-order nonlinear optical chromophore is prepared through treating a 1,1,7,7-tetramethyljulolidine derivative as an electron donor and tricyanodihydrofuran or tricyanopyrroline as an electron acceptor. The alkyl group on the julolidine donor N used in the synthetic method and a phenyl ring form a closed six-membered ring, and the upper surface and the lower surface of the six-membered ring are respectively connected with a methyl group, so the spatial steric hindrance structure can effectively reduce the interaction force among molecules and improve the first-order molecular hyperpolarizability (beta) of the molecules of the chromophore. The organic second-order nonlinear optical chromophore having the D-pi-A structure can be doped with an amorphous polycarbonate to prepare a polarized polymer film, and the prepared film can be used as a material in the optical signal modulation field. The structures of the organic second-order nonlinear optical chromophore are represented by formulas in the specification.