Piezoelectric nanogenerators (PENGs) are booming for energy collection and wearable energy supply as one of the next generations of green energy-harvesting devices. Balancing the output, safety, degradation, and cost is the key to solving the bottleneck of PENG application. In this regard, yttrium (Y)-doped zinc oxide (ZnO) (Y-ZnO) was synthesized and embedded into polylactide (PLLA) for developing degradable piezoelectric composite films with an enhanced energy-harvesting performance. The synthesized Y-ZnO exhibits high piezoelectric properties benefiting from the stronger polarity of the Y-O bond and regulation of oxygen vacancy concentration, which improve the output performance of the composite film with Y-ZnO and PLLA (Y-Z-PLLA). The obtained open-circuit voltage ( V oc ), short-circuit current ( I sc ), and instantaneous power density of the optimized Y-Z-PLLA PENG reach 17.52 V, 2.45 μA, and 1.76 μW/cm 2 , respectively. The proposed PENG also shows good degradability. In addition, practical applications of the proposed PENG were demonstrated by converting biomechanical energy, such as walking, running, and jumping, into electricity.