Polymer-based magnetoelectric composite materials have attracted a lot of attention due to their high potential in various types of applications as magnetic field sensors, energy harvesting, and biomedical devices. Current researches are focused on the increase in the efficiency of magnetoelectric transformation. In this work, a new strategy of arrangement of clusters of magnetic nanoparticles by an external magnetic field in PVDF and PFVD-TrFE matrixes is proposed to increase the voltage coefficient (α_ME) of the magnetoelectric effect. Another strategy is the use of 3-component composites through the inclusion of piezoelectric BaTiO₃ particles. Developed strategies allow us to increase the α_ME value from ~5 mV/cm·Oe for the composite of randomly distributed CoFe₂O₄ nanoparticles in PVDF matrix to ~18.5 mV/cm·Oe for a composite of magnetic particles in PVDF-TrFE matrix with 5%wt of piezoelectric particles. The applicability of such materials as bioactive surface is demonstrated on neural crest stem cell cultures.