A nonlinearity in the magnetoelectric coefficient, alpha(Nonlin)(ME), of Metglas/Pb(Zr,Ti)O(3) (PZT) and Metglas/Pb(Mg(1/3),Nb(2/3))O(3)-PbTiO(3) (PMN-PT) laminate sensors has been observed. This nonlinearity was found to be dependent on the dc magnetic bias (H(dc)) and frequency of the ac drive field (H(ac)). The maximum value of alpha(Nonlin)(ME) for both types of composites was found near the electromechanical resonance. For Metglas/PZT laminates, the maximum occurred under a finite bias of H(dc) approximate to 5 Oe; whereas, for Metglas/PMN-PT, the maximum was found near zero dc bias. One application for alpha(Nonlin)(ME) is a cross-modulation scheme that can shift low frequency signals to higher frequency to achieve lower noise floor. For Metglas/PMN-PT, alpha(Nonlin)(ME) has another application: removal of the necessity of a dc bias, which helps to design high-sensitivity sensor arrays and gradiometers. (C) 2011 American Institute of Physics. [doi:10.1063/1.3665130]