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An electro-optic modulation system was adopted for measuring the quadratic electro-optic coefficient of KTN crystal. Theoretical analysis and experimental results verified the feasibility of this method. The quadratic electro-optic coefficient of a KTN crystal chip, which has a Curie temperature of 0 °C, was measured using this system in the temperature range of 2 °C to 18 °C (T_c = 0 °C). The influences of temperature, AC voltage and frequency on the quadratic electro-optic coefficient were discussed. It was found that the relaxation effect of PNRs (polar nano-regions) played an important role in the determination of the quadratic electro-optic coefficient of KTN crystal.