“…The initial work on composite multiferroics was developed at the Philips Research Laboratories in the 1970s and was aimed at designing composite ceramics by either exploring the phase stability diagram of the quinary system Fe–Co–Ti–Ba–O to produce an aligned two‐phase composite of ferroelectric BaTiO 3 and magnetic (CoFe 2 O 4 ) 1‐ x (Co 2 TiO 4 ) x oxides,127, 154, 155 or more simply by sintering ferroelectric and ferromagnetic powders to achieve the composite structure 156, 157. The magnetoelectric coupling coefficients characteristic of these composites were larger than those typical of intrinsic multiferroics, in the range from 1–130 mV cm −1 Oe −1 , but the magnetoelectric coupling depended strongly on the exact composition of the magnetic phase, crystallite size, and grain arrangement, giving rise to a large variability in properties 128, 152, 157–159. Other difficulties relate to electrical shunting from the low resistivity magnetic component (limiting the electric field strength used for poling and resulting in the loss of induced voltage);160, 161 residual strain or cracks that may develop during thermal cycling due to thermal expansion mismatch between phases, leading to poor mechanical coupling; the presence of voids and spurious phases; defects in the crystalline structure of each phase, including vacancies and dislocations; variations in crystallite sizes, shapes, and packings, which can reduce the mechanical coupling; deviations from bulk properties, such as reduced magnetic and electric polarizations, reduced magnetostrictive and piezoelectric coefficients, modified magnetic anisotropies, and dielectric response; and the presence of magnetic and ferroelectric domain walls 128, 162–163…”