Nature has created a wide range of hierarchical materials, including nanostructured biological materials like wood, which are formed by assembling repetitive building blocks into higher-order architectures. This hierarchical design gives wood exceptional properties, attributed to its renewable origin, easy surface chemical modification, and favorable mechanical properties, urging its multi-functionalization for various applications through bio-inspired multiscale assembly approaches. Reinventing its traditional background, wood is emerging as an ideal candidate for sustainable piezoelectric mechanical energy harvesting devices. In this work, (r)evolutionizing piezoelectric nanogenerators (PENGs), an innovative and scalable method for developing environmentally friendly Wood/ZnO multifunctional composites with piezoelectric performance, is proposed. Starting by strategically combining delignification and position-selective oxidation, via periodate – or TEMPO – mediated oxidation, the porous oxidized wood templates (WTs) were further impregnated with multilayered ZnO morphologies through hydrothermal synthesis (Wood/ZnO). Controlled ZnO nanorods were achieved, enabling tunable piezoelectric outputs through the novel combination of seed-layer pre-fabrication and precursor infiltration. Finally, Wood/ZnO PENGs with anisotropic piezoelectric performance were prepared by impregnating Wood/ZnO with PDMS (Wood/ZnO elastomer), exhibiting unique mechanical robustness and efficient mechanical energy conversion, while preserving wood’s hierarchical structure. Position-selective oxidation process and in-situ ZnO growth have proven to be critical to enhancing the piezoelectric response. Therefore, Wood/ZnO elastomer PENGs demonstrated significantly higher output voltages compared to their Wood/ZnO composite PENGs counterparts, maintaining stable performance under cyclic mechanical compression. Wood/ZnO elastomer from neutral TEMPO oxidation (WZE_T) stood out for its remarkable cell wall flexibility and mechanical resilience, achieving an output voltage of 16.96 V and current of 14.20 µA – surpassing the performance of previously reported Wood/ZnO PENGs. Wood nanotechnology is at the frontier of sustainable innovation. The proposed scalable method, combined with Wood/ZnO PENGs piezoelectric performance, highlights the potential for designing advanced wood nanocomposites towards efficient energy harvesting systems, while leveraging wood’s outstanding features and natural architectures.