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Magnetoelectric (ME) (100-
x
) Na
0.5
Bi
0.5
TiO
3
(NBT)–
x
CoFe
2
O
4
(CFO) (
x
= 30 and 35) particulate composites were prepared from the pre-sintered individual constituents by adopting mixed oxide route. The composites consisting of CFO grains embedded in a twice-grain-sized NBT matrix were investigated for the enhancement of the ME coefficient. CFO grains are not interlinked which implied that composites are within percolation limit and thereby 0–3 particulates are formed without impurity phase at the interface is evidenced by XRD, SEM micrographs and elemental mapping. Raman modes due to the influence of CFO are visible around 213 cm
−1
. A non-saturated PE loop indicates leaky behavior and the MH loop depicts the magnetic behavior of samples. ME coefficient is 18.9 mV/cm Oe for the 65NBT-35CFO composite and it is higher than that reported in the NBT–CFO composites. Theoretical modeling of the ME coefficient signifies that the observed experimental value is much smaller than the theoretical value.