A series of three-phase composite films with different filler contents were prepared by in-situ polymerization. The composite films comprise polyimide (PI), poly (vinylidene fluoride) (PVDF), and titanium dioxide (TiO2). Compared with PI/TiO2 composite films, the PI/TiO2-PVDF composite films not only get a significant increase in dielectric constant, but also own better mechanical properties. Our results show that with the loading of 50wt% PVDF particles, the dielectric constant of PI/TiO2-PVDF composite films increased from 6.5 to 18.14 at 1 MHz and room temperature, while the tensile strength of PI/TiO2-PVDF composite films increased from 45 to 72 MPa. In addition, the films maintain a low loss tangent of about 0.02. PI/PVDF composite films were also prepared. It was found that dielectric constant of PI/PVDF composite was significantly lower than that of PI/TiO2-PVDF composite films when the loading of PVDF is 50wt%.
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