Enhanced Magnetoelectric Coupling in Lead‐Free BaZr 0.05 Ti 0.95 O 3 ‐0.5Ba 0.92 Ca 0.08 TiO 3 Piezoelectric and Ni 0.8 Co 0.2 Fe 1.95 (Dy 0.7 Tb 0.3 ) 0.05 O 4 Magnetostrictive Composites

Magnetoelectric (ME) materials, which exhibit coupling between magnetic and ferroelectric order, hold promise for advanced electronic and energy‐harvesting applications. This study investigates a novel lead‐free ME composite system comprising Ni 0 . 8 Co 0 . 2 Fe 1 . 95 (Dy 0 . 7 Tb 0 . 3 ) 0 . 0 5 O 4 as the magnetostrictive phase and BaZr 0 . 0 5 Ti 0 . 9 5 O 3 ‐0.5Ba 0 . 9 2 Ca 0 . 0 8 TiO 3 as the piezoelectric phase. The effects of magnetostrictive phase content on the structure, microstructure, magnetic, piezoelectric, dielectric, ferroelectric, and ME properties are systematically evaluated. X‐ray diffraction and Raman spectroscopy confirm the tetragonal perovskite structure of the ferroelectric phase and the spinel cubic structure of the magnetic phase, while scanning electron microscopy reveals a dense microstructure (1.17 to 1.62 μm). Magnetic measurements at 5 K and 300 K exhibit well‐saturated hysteresis loops with low coercivity, indicative of soft ferrimagnetism. Ferroelectric hysteresis ( P – E ) loops indicate that the M1 and M2 composites retain typical ferroelectric characteristics, with the M2 composite exhibiting a notable remnant polarization of 4.70 μC cm − 2 . The M3 composite shows a squareness ratio of 0.66, suitable for multistate memory applications. The M1 composite exhibits a piezoelectric coefficient of 112 pC/N and an ME coefficient of 187.1 mV/(cm‐Oe), making it suitable for magnetic field sensing. These results highlight the potential of lead‐free ME materials for next‐generation energy, sensing, and memory applications.