Simple and cost-effective procedures for the direct integration of ferroelectric perovskite oxides into Ni structures are necessary to realize related multifunctional metallic microelectromechanical systems, such as dual-source energy harvesters. This is especially difficult in the case of lead-containing morphotropic phase boundary materials for high piezoelectric response because the two components are thermodynamically incompatible and the formation of NiOx or perovskite oxide reduction takes place depending on the processing conditions. We show here that low-temperature solution processing is an effective means to kinetically limit nickel oxidation, capable of providing BiFeO3–PbTiO3 films on Ni plates at only 500 °C. Bulk-like ferroelectric properties and a distinctive magnetoelectric response were attained. This perovskite system, not explored before on Ni, has a much larger switchable polarization than the widely studied Pb(Zr,Ti)O3, and it is shown here to present an excellent downscaling behavior of ferroelectric properties until the verge of the nanoscale.