Na0.5Bi0.5TiO3 (NBT), CoFe2O4 (CFO) as well as particulate composites containing different mole percentages of NBT and CFO were synthesized by the solid-state sintering route and characterized for their ferroelectric and ferrimagnetic hysteresis loops, magnetostriction and magnetoelectric (ME) output. The mole% of CFO was found to influence the ferroelectric and ferrimagnetic hysteresis loops as well as magnetostriction and piezomagnetic coefficients which in turn had a significant effect on the magnetoelectric voltage coefficient. The highest magnetoelectric voltage coefficient (α) of 0.5mV/cm/Oe was recorded in (65) NBT–(35) CFO composite.