a b s t r a c t The synthesis and nonlinear optical (NLO) properties of a series of nitrostilbene-, dinitrostilbene-, and dicyanomethylenedihydrofuran-based chromophores potentially useful in photorefractive multifunc-tional polymers are reported. Electronic absorption spectra have been measured in different solvents. Electric field induced second harmonic (EFISH) generation results show that the 2-dicyanomethylen-3-cyano-5,5-dimethyl-2,5-dihydrofuran moieties lead to the best NLO performances. Dinitrophenyl-based chromophores have shown a reduced nonlinear response as compared with the mononitro analogues. Nonlinear optical properties of a selected nitro–dinitro couple have been also determined theoretically.