Engineering ZnO/CuO Heterojunctions via Supramolecular Mediation Leading to Morphology‐Dependent High‐Performance Piezoelectric Catalyst

Abstract Piezoelectric catalysis, utilizing mechanical energy to generate reactive oxygen species (ROS), has emerged as a promising strategy in environmental remediation. However, developing high‐performance piezocatalysts operable under low‐frequency conditions remains a huge demand and challenge. Herein, an innovative supramolecular‐driven hydrothermal strategy is proposed for precise morphology regulation and synthesis of ZnO/CuO piezocatalysts. Using self‐assembled natural betulinic acid as a dynamic soft template, four types of ZnO/CuO heterojunctions are successfully synthesized with progressively tuned morphologies, including rod‐like (RPs), airship‐like (APs), star‐like (SPs), and urchin‐like (UPs) particles, which exhibit enhanced sharp protrusions and highly bendable features. Structural modulation and ROS mechanistic analyses reveal a distinct piezoelectric trend of UPs > SPs > APs > RPs. This implies that higher strain probability or larger strain gradients, resulting from increased sharp protrusions, lead to improved piezoelectric performance. Significantly, the UPs exhibit exceptional piezocatalytic activity under low‐frequency mechanical stirring, achieving a degradation rate constant of 40.8 × 10 ⁻³ min ⁻¹ for dye rhodamine and an 88.4% bacterial inhibition rate at merely 60 ng mL ⁻¹ . This work not only provides a promising option for the application of commercial high‐performance piezocatalysts in environmental regeneration but also highlights the potential of supramolecular‐mediated morphology regulation strategies for designing advanced piezocatalysts adapted to diverse applications.