Abstract Two-phase magnetostrictive–piezoelectric thin film composites are key materials to the development of a range of potentially disruptive magnetoelectric technologies, such as electrical-writing magnetic-reading random access memories. However, multiferroic thin film composites prepared so far show neither magnetoelectric switching nor magnetoelectric responses comparable to those of related bulk ceramic materials and cermets. Here we show that ion implantation of magnetic species into ferroelectric single crystal targets can be an effective alternative means of obtaining nanoparticulate thin film composites of this type. Concept is proved by the implantation of Co into a Pb(Mg_1/3Nb_2/3)O₃–PbTiO₃ single crystal with ultrahigh piezoelectricity. Formation of an ensemble of ferromagnetic nanoparticles embedded in an amorphized layer within the ferroelectric crystal is clearly shown.