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Novel nonlinear optical (NLO) chromophore using benzo[b]furan moiety and trifluoromethyl-substituted tricyanofuran as the electron donor and acceptor respectively was designed and prepared. The structure of the novel chromophore was determined by NMR spectra, and the photophysical properties were studied via UV-vis spectra. The thermal decomposition temperature (T d)value of the obtained NLO chromophore reached to 212 °C, which endow the chromophore with good thermal stability during the materials processing. The nonlinearity of the chromophore was evaluated through theoretical calculation and electro-optic (EO) activity test, and the highest EO coefficient (r 33) was determined to 28 pm/V at the loading density of 25 wt% in polymethyl methacrylate. • Novel benzofuran-based nonlinear optical chromophore was designed and synthesized. • The acceptor was unexpected linked to the β -position of furan in the chromophore. • The present chromophore exhibited go0d thermal stability (T d reached to 212 °C). • The maximum EO coefficient of the reported chromophore reached to 28 p.m./V. [ABSTRACT FROM AUTHOR]