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Orderly polymer composites based on polyvinylidene fluoride assembled with parallel aligned zinc flakes were fabricated by a simple process. It is interesting to note that the microstructure of parallel arrangement could introduce excellent dielectric properties with obvious anisotropic dielectric behaviors. The dielectric constant in the parallel direction was obviously higher than that of the perpendicular direction. And the anisotropic intensity of interfacial polarization is proposed to interpret the anisotropic dielectric constant. Also, an equivalent circuit model of two parallel RC circuits in series, based on the analysis of impedance data, is employed to further discuss the anisotropic dielectric behavior.