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A piezoelectric polymer multilayer structure formed on a flexible substrate is investigated for mechanical energy harvesting under bending mode. Analytical and numerical models are developed to clarify the effect of material parameters critical to the energy harvesting performance of the bending multilayer structure. It is shown that the maximum power is proportional to the square of the piezoelectric stress coefficient and the inverse of dielectric permittivity of the piezoelectric polymer. It is further found that a piezoelectric multilayer with thinner electrodes can generate more electric energy in bending mode. The effect of improved impedance matching in the multilayer polymer on energy output is remarkable. Comparisons between piezoelectric ceramic multilayers and polymer multilayers on flexible substrate are discussed. The fabrication of a P(VDF-TrFE) multilayer structure with a thin Al electrode layer is experimentally demonstrated by a scalable dip-coating process on a flexible aluminum substrate. The results indicate that it is feasible to produce a piezoelectric polymer multilayer structure on flexible substrate for harvesting mechanical energy applicable for many low-power electronics.