Nontoxic lead-free multiferroic composites are synthesized by incorporating the dispersed 0.3 CoFe 2 O 4 (CFO) ferromagnetic nanoparticles into 0.7( K 0.5 Na 0.5) NbO 3- LiSbO 3 (KNN-LS5.2) ferroelectric micromatrix. The multiferroicity of the composite can be verified by polarization-electric field hysteresis loop and magnetic hysteresis loop. The composite exhibits excellent magnetic properties. A dilution effect is observed in magnetic hysteresis loops. The field dependence of ME voltage coefficient is given as a function of magnetic field from -4 kOe to 4 kOe with a maximum magnetoelectric voltage coefficient of 10.7 mV ⋅ cm -1⋅ Oe -1 at the frequency of 1 kHz. It is a very high value in the lead-free magnetoelectric composites system for the potential use on multifunctional devices.