Nanohybrid structures of FePt and BaTiO₃ with bifunctional properties were synthesized by a two step synthesis procedure including solid state and solvothermal methods. Two different compositions of FePt and BaTiO₃ nanoparticle samples were synthesized. The hybrid composite, having the lower FePt concentration, exhibited bifunctionality including superparamagnetism with a blocking temperature near room temperature and ferroelectricity at ambient conditions. Magnetocapacitive measurements of this bifunctional FePt–BiTiO₃ sample showed behaviour typical of weak magnetoelectric coupling. This synthetic approach provides a general method for preparing advanced multifunctional and technologically important ceramic–alloy hybrids.