High-entropy oxides provide a powerful platform for engineering mechanically driven catalysis, yet their underlying mechanisms remain poorly understood. Here, we investigate the catalytic performance of high-entropy perovskites, Sr(Ti, Zr, Hf, Sn, Nb)O3 (STZHSN) and Pb(Mg, Nb, Zr, Ti, Hf)O3 (PMNZTH), alongside single-component oxides SrTiO3 (STO) and BiFeO3 (BFO), revealing a clear correlation between compositional complexity and activity. PMNZTH exhibited the highest catalytic efficiency, followed by STZHSN and STO, with BFO performing the least effectively. Using combined ultrasonic and blade-induced agitation, we show that fluid turbulence and solid–liquid interfacial dynamics critically enhance charge transfer. Spectroscopic and theoretical analyses indicate that surface hydroxyl groups facilitate the formation of reactive oxygen species, while cavitation and friction drive a self-sustaining redox cycle. These insights culminate in a unified surface-electrostatics-driven catalysis model, where interfacial surface potential, hydroxyl adsorption, and turbulence-enhanced charge transport govern the activity beyond intrinsic piezoelectric effects. This study establishes high-entropy design as a versatile strategy for optimizing mechanically driven catalysts for energy conversion and environmental remediation.
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