Measurements are presented of the magnetoelectric (ME) coupling of nontoxic lead-free multiferroic composites 0.4CoFe2O4-0.6[0.948(K0.5Na0.5)NbO3-0.052LiSbO3]. The composites are found to exhibit an interesting dielectric response under a dc magnetic bias field. The positive magnetodielectric behavior and its strong frequency dependence in the composite could be related to magnetoresistance and the Maxwell-Wagner effect. The ME effects are strongly dependent on the driving field frequency and dc magnetic bias field. The frequency and magnetic field dependence of direct and converse ME coefficients are related to the relative dielectric constant and the variation in the piezomagnetic coupling with magnetic field, respectively. In addition, the dependence of direct and converse ME coefficients on frequency and magnetic field is quite similar in this multiferroic particulate composite.