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The piezoelectric nanogenerator (PENG) has the potential to become a promising power supply for monitoring and sensors in Internet of Things (IoT) systems through wireless networks. In order to further increase the utilization of energy harvesters in an IoT system, we introduce a novel approach that greatly enhances the piezoelectric output performances by employing the layer-by-layer (LbL) method. Poly(vinylidenefluoride-co-trifluoroethylene) (PVDF-TrFE) polymer film, which has piezoelectric properties and mechanical flexibility, was used for the active layer in PENG. The maximum open-circuit voltage and closed-circuit current of the LbL multilayer PENG reached 34 V and 100 nA, respectively. In particular, the closed-circuit current of the LbL multilayer PENG was dramatically improved to be five times higher than that of the single-layer PENG. Furthermore, a supercapacitor was employed to investigate the energy storage capability of PENGs using different methods. The proposed LbL multilayer PENG is expected to be a candidate for a promising power supply for self-powered systems in the IoT system. [ABSTRACT FROM AUTHOR]