In this paper, giant resonant magnetoelectric (ME) effect in an unsymmetrical bi-layered Metglas/Pb(Zr,Ti)O-3 ME composites with multi-push pull configuration that can be significantly tuned was investigated experimentally and theoretically. The actual measured and predicted results present the similar resonant frequency shifting behaviors for such ME composites: The resonant frequency can be varied from 70 Hz to 220 Hz by tip mass loading, where the ME voltage coefficients were over 250 V/cm-Oe. Moreover, the giant frequency-tunable resonant effect allowed us to design a 60Hz magnetic field energy harvester to be capable of harvesting energy generated by electronic instruments working on a 60Hz ac power supply. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4765724]