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Dense α-phase blend films of vinylidene fluoride (VDF) oligomer and poly(vinylidene fluoride) (PVDF) of various compositions were prepared from chemical solution deposition. The dielectric constant of the films was unexpectedly lower, and the mechanical strength was higher than either of the two components, leading to high electromechanical dielectric breakdown strength (>850 MV/m vs. 300∼500 MV/m for typical PVDF-based films). The properties were attributed to the unique blend structure with high crystallinity and densely packed rigid amorphous phase incorporating long and short chains. A maximum polarization of 162 mC/m2 and a large electric energy density up to 27.3 J/cm3 were obtained.