This work examines the potential of PbZr 0.53 Ti 0.47 O 3 /CoFe 2 O 4 (PZT/CFO) multi-layered nanostructures (MLNs) for giant electrocaloric effect (ECE) and pyroelectric energy harvesting.Unlike the conventional ECE, the presented MLNs is governed by the dynamic magneto-electric coupling (MEC) and can be tuned by the arrangement of the various ferroic layers. The ECE in alternate layers of PZT and CFO in a stack of three (L3), five (L5) and nine (L9) alternating PZT and CFO layers are investigated. An ECE temperature change of 52.3 K, 32.4 K and 25.0? K is predicted in these MLNs respectively. Intriguingly, all configurations exhibit a negative ECE which has a high magnitude in comparison with previously reported giant negative ECE (|∆T|=6.2 K) 1, 2 . In addition, the maximum indirect pyroelectric energy harvesting obtained from these layers using a modified Olsen cycle is four times higher than the highest reported pyroelectric energy density of 11549 kJm -3 cycle -1 3, 4 . This increase is attributed to the cumulative effect of multiple layers that induce an enhancement in the overall polarization (1.5 times of lead zirconate titanate) and leads to abrupt polarization changes with a temperature fluctuation. The present study also sheds light on materials selection and the thermodynamic processes involved in the ECE. It is concluded that the refrigeration obtained from reversed Olsen cycle is a combined effect of an isothermal entropy as well as adiabatic temperature change.