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Nickel niobate (NiNb2O6) was used to modify the barium titanate (BaTiO3) ceramics, the obtained NiNb2O6‐BaTiO3 ceramics possess better dielectric performances than that of raw BaTiO3. By adding NiNb2O6‐BaTiO3 into poly(arylene ether nitriles) (PEN) polymer, a series of NiNb2O6‐BaTiO3/PEN composite films with different NiNb2O6‐BaTiO3 contents were prepared via solution casting method. The morphology, thermal, mechanical, dielectric properties, and flexibility of the obtained NiNb2O6‐BaTiO3/PEN composite films were investigated detailedly. As the filler content increases, the tensile modulus of NiNb2O6‐BaTiO3/PEN composite films increases gradually, while the tensile strength decreases. Thermal and flexibility analysis shows that the addition of the NiNb2O6‐BaTiO3 fillers does not affect the thermal and flexibility properties endowed by the PEN matrix. The dielectric constant of the composites almost linearly increases from 3.7 (1 kHz) to 15.3 (1 kHz) as the filler content increases from 0 to 40 wt%. Besides, results show that NiNb2O6‐BaTiO3/PEN composites exhibit higher dielectric constant than that of BaTiO3/PEN. The as‐prepared NiNb2O6‐BaTiO3 will be a more promising filler to prepare polymer‐ceramic composites for organic film capacitors. [ABSTRACT FROM AUTHOR]