Here, we report exotic role of electrical poling of layered BCZT-CNZF bulk composite for a sustainable advancement of magnetoelectric (ME) technology. Practically, it seems quite difficult to access full potential of ME composites due to their weak ME coupling performances. Using a standard poling protocols, we successfully deployed coupling performance of laminated ME composite, comprises of ferroelectric (FE) layer of BCZT and a ferrite layer of CNZF. However, the ME coupling constant of laminated composite is optimized by lowering volume fraction of FE component to strengthen the mechanical strain in piezoelectric layer, while fixing the thickness of the magnetostrictive ferrite layer. Here, we employed systematic zero field cooled (ZFC) and field cooled (FC) electrical poling protocol on morphotropic phase boundary (MPB) based BCZT composition, well-appreciated for it’s remarkable electromechanical activity. We report a record augmentation in magnetoelectric coupling as a consequence of prudent field cooled poling mechanism. On the basis of our findings, we emphasize that the degree of magnetoelectricity may be significantly improved for miniaturization of efficient devices via proper execution of poling technique.