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Lately, polymer based piezoelectric materials that harness energy from mechanical vibrations and/or impact are being increasingly investigated as radical alternates to conventional batteries that are hard to service once deployed. Nevertheless, the optimization of energy outputs of piezoelectric energy harvesters is one of the prime challenges faced by the scientific community. This chapter provides an overview of polymer based piezoelectric energy harvesters with special emphasis on current state of research on polymer composites/nanocomposites for vibrational energy harvesting. A detailed summary of piezoelectric phenomenon in polymers is also presented. An in-depth narration detailing the enhancement of piezoelectric behavior of one of the most commonly employed piezoelectric polymer (PVDF) is presented with special emphasis on some of the promising filler materials towards realizing high efficient piezoelectric modules. This chapter is intended to give an insight on the recent advances in the field of polymer based piezoelectric materials.