Flexible magnetoelectric (ME) nanocomposites with a strong coupling between ferromagnetism and ferroelectricity are of significant importance from the point of view of next-generation flexible electronic devices. However, a high loading of magnetic nanomaterials is needed to achieve preferable ME response due to the size mismatch of the magnetostrictive phase and piezoelectric phase. In this work, ultra-small CoFe2O4 nanoparticles were prepared to match the size of the polar crystal in poly(vinylidene fluoride-trifluoroethylene) (P(VDF-TrFE)), and 1H,1H,2H,2H-perfluorooctyltriethoxysilane (POTS) is introduced to enhance the interplay between P(VDF-TrFE) and CoFe2O4. The above multiple effects promote a good connection between the magnetostrictive phase and the piezoelectric phase. Therefore, an effective transference of stress from CoFe2O4 to P(VDF-TrFE) can be achieved. The as-prepared P(VDF-TrFE)/CoFe2O4@POTS exhibits a high ME coupling coefficient of 34 mV cm-1 Oe-1 when the content of CoFe2O4@POTS is 20 wt%. The low loading of fillers ensures the flexibility of ME nanocomposite films.