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Based on the principles of molecular engineering, a series of new chromophores with high second-order nonlinear optical(NLO)activities have been designed for achieving a trade-off of the nonlinearity-transparency-thermal stability. The NLO properties of these chromophores have been investigated theoretically by employing the AMI/Finite Field approach. It is found that the calculated μβ0 values of some designed chromophores can reach the magnitude of 10-45 esu, and the highest decomposition temperature Td can be as high as 377℃, the highest glass transition temperature Ts of their donor-embedded addition-type polyimides can be as high as 324℃.