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• Novel FTC-type NLO chromophore is designed to developing high performance EO material. • The obtained NLO chromophore possesses good film forming ability and obvious T g near 75 °C. • As EO molecular glass, the poled pure chromophore film displayed the r 33 value of 160 pm/V. To explore the simple strategy for developing excellent electro-optic (EO) materials, a monolithic EO molecular glass (EOMG1) based on thiophene π-conjugation and tricyanofuran acceptor (FTC) was synthesized. A tert -butyldiphenylsilyl (TBDPS) group was introduced to the FTC-based nonlinear optic (NLO) chromophore. The glass transition temperature (T g) of the amorphous films was near 75 ℃, confirmed EOMG1 's glassy state. The theoretical calculation shows that the first hyperpolarizability (β) and dipole moment (μ) of EOMG 1 were calculated to 584 × 10−30esu and 20.73 D. After poling, the poled films EOMG1 diplay large EO activity (r 33) of 160 pm/V at 1310 nm. The r 33 value is greatly enhanced compared to the reported side-chain EO polymer containing the similar FTC-type NLO chromophore due to the increased loading density of the pure chromophore films and the TBDPS group's role of effective isolation. [ABSTRACT FROM AUTHOR]