The electro-optic crystal holds great promise for extensive applications in optoelectronics and optical communication.However,the discovery of novel electro-optic crystals is sporadic due to the difficulties of large-sized crystal growth for electro-optic coefficient measurement.Herein,to address this issue,a high-efficacy evaluation method using accessible powder samples is proposed in which the second-harmonic-generation effect,infrared reflectance spectrum and Raman spectrum are introduced to predict the magnitude of the electro-optic coefficient.The calculated electro-optic coefficients of numerous reported electro-optic crystals through this approach give universal agreement to the experimental values,evidencing the validity of the strategy.Based on this method,CsLiMoO4 is screened as a novel potential electro-optic crystal and a high-quality crystal is grown by the Czochralski technique for electro-optic coefficient measurement using the half-wave voltage method,the result of which is also comparable to the calculated value.Consequently,the evaluation strategy presented here will pave a new way to explore promising electro-optic crystals efficiently.