Zeolites with framework types LTL, LTA, FAU, and MFI were synthesized and used as fillers to prepare PVDF/zeolite composites. The obtained composites showed structural and electrical dependence on the pore system and chemical content of the inorganic host. The larger polymer-zeolite electrostatic interactions of the Y and A zeolites lead the polymer to crystallize in the electroactive gamma-phase, which in the case of the L zeolite is prevented due to the reduced interaction area. The solvent and water encapsulation ability of the zeolite as well as improve of the dielectric response of the composite is directly related to the Si/Al ratio, leading zeolites with lower Si/Al ratios to larger dielectric responses and encapsulation efficiencies in the composites. These effects show also some dependency on the dimensionality of the pore system; the zeolite L-containing 1D channels showing superior dielectric performance than the 3D pore system of zeolite Y.