A polymer composite was prepared by embedding fillers made of self-passivated aluminum particles in two kind of sizes, micrometer size and nanometer size with different volume proportions into polyvinylidene fluoride matrix. The thermal conductivity and dielectric properties of the composite were studied. The results showed that the thermal conductivity of composites was significantly increased to 3.258 W∕mK when the volume proportion of micrometer size Al particles to nanometer size Al particles is at 20:1, also the relative permittivity was about 75.8 at 1 MHz. The effective simulation model values were in good accordance with experimental results.