Magnetoelectric microspheres based on piezoelectric poly(vinylidene fluoride) (PVDF) and magnetostrictive CoFe 2 O 4 (CFO), a novel morphology for polymer-based ME materials, have been developed by an electrospray process. The CFO nanoparticle content in the (3-7 mm diameter) microspheres reaches values up to 27 wt%, despite their concentration in the starting solution reaching values up to 70 wt%. Additionally, the inclusion of magnetostrictive nanoparticles into the polymer spheres has no relevant effect on the piezoelectric b-phase content (z60%), crystallinity (40%) and the onset degradation temperature (460-465 C) of the polymer matrix. The multiferroic microspheres show a maximum piezoelectric response |d33| z 30 pC N1, leading to a magnetoelectric response of D|d33| z 5 pC N1 obtained when a 220 mT DC magnetic field was applied. It is also shown that the interface between CFO nanoparticles and PVDF (from 0 to 55%) has a strong influence on the ME response of the microspheres. The simplicity and the scalability of the processing method suggest a large application potential of this novel magnetoelectric geometry in areas such as tissue engineering, sensors and actuators. Magnetoelectric microspheres based on piezoelectric poly(vinylidene fluoride) (PVDF) and magnetrostrictive CoFe 2 O 4 (CFO), a novel morphology for polymer-based ME material, have been developed by an electrospray process. The CFO nanoparticles content in the (3 -7 µm diameter) microspheres reaches values up to 27 wt.%, despite their concentration in the starting solution reaching values up to 70 wt.%. Additionally, the inclusion of magnetostrictive nanoparticles into the polymer spheres has no relevant effect on the piezoelectric β-phase content (≈60%), crystallinity (40%) and the onset degradatio n temperature (460º-465ºC) of the polymer matrix. The multiferroic microspeheres show a maximum piezoelectric reponse |d33|≈30 pC.N -1 , leading to a magnetoelectric response of ∆|d33|≈5 pC.N -1 obtained when a 220 mT DC magnetic field was applied. It is also shown that the interface between CFO nanoparticles and PVDF (from 0 to 55%) has a strong influence on the ME response of the microspheres. The simplicity and the scalability of the processing method suggest a large application potential of this novel mag netoelectric geometry in areas such as tissue engineering, sensors and actuators.