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The CoFe2O4-BaTiO3 core-shell (CFO@BTO) nanocomposites have been synthesized, and a particular volume fraction of 15% CoFe2O4–85% BaTiO3 has been studied for its magnetic, ferroelectric, and magnetoelectric properties. The optimization of synthesis conditions showed that a temperature of at least 800 °C is required to obtain pure phase BaTiO3, whereas for the tetragonality to be visible in the x-ray diffraction (XRD) pattern, BaTiO3 needed to be sintered to at least 1050 °C. Even though the CFO@BTO composite began to react at the interface at 1050 °C and a small amount of the secondary phase was observed in the XRD pattern, the ferroelectric and magnetic properties were found to be not affected. Upon treating the living epithelial cells with either CFO@BTO or BTO nanoparticles, no toxicity was observed for up to 7 days. Together, these results establish the potential for the use of CFO@BTO nanoparticles in biomedical applications. [ABSTRACT FROM AUTHOR]