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Crystalline silica was synthesized by annealing amorphous silica at 1,300℃ or 1,400℃ for various times, and the crystallinity was estimated by X-ray diffraction (XRD) analysis. In order to prepare a low dielectric material, epoxy/crystalline silica composites were prepared, and the effect of silica content on the dielectric properties was studied under various functions of frequency and ambient temperature. The dielectric constant decreased with increasing crystalline silica content in the epoxy composites, and it also decreased with increasing frequency. At 120 Hz, the value of 5 wt% silica decreased by 0.25 compared to that of 40 wt% silica, and at 23 kHz, the value of 5 wt% silica decreased by 0.23 compared to that of 40 wt% silica. The value increased with increasing ambient temperature.