Owing to the hierarchical structure, easy multi-functionalization and favorable mechanical properties, wood could harvest electricity from mechanical energy through piezoelectric behavior. In this work, a scalable method to synthesize wood/ZnO composite with multilayered ZnO morphologies is reported for efficient mechanical energy conversion. The synthesis includes charged wood template fabrication, precursor infiltration, and ZnO hydrothermal growth, resulting in controlled ZnO morphologies and distributions while maintaining the hierarchical structure of the wood. Stereo-digital image correlation (stereo-DIC) investigated the relationship between deformation and piezoelectric performance, which revealed the homogeneous distribution of multilayered ZnO enhance piezoelectric performance. The output voltage of wood/ZnO was 1.5 V under periodic mechanical compression (8–10 N) for 300 cycles, while the output current was 2.91 nA. The scalable synthesis strategy and piezoelectric performance are significant for the design of advanced wood nanocomposites for sustainable and efficient energy conversion systems.