Two-phase hybrid fillers of BaTiO3(BT) and carbon nanotube (CNT) with three inter structures but same volume ratios were loaded into polyvinylidene fluoride (PVDF) matrix. Three inter structures of two-phase hybrid fillers were simple mechanical mixing, CNT growing on the surface of BT particles by chemical vapor deposition (CVD) and BT coating on the CNT surface by hydrothermal, respectively. An obvious diversity of dielectric properties and percolation phenomenon for the three composites was observed when with the same fillers volume fraction. The difference among inter structures of the two-phase hybrid fillers and interfaces would result in the diversity of the dielectric properties of composites.