Photodetectors In article number 2101263, Jianhua Hao and co-workers report the use of ferroelectric EA4Pb3Br10 single-crystalline thin-films to broaden perovskite photodetection applications with piezo-phototronic effect enhanced behavior. The coupling of ferroelectric spontaneous polarization and the piezoelectric effect, as well as photoexcitation and semiconductor behaviors endow the EA4Pb3Br10-based flexible photodetectors with a strain-modulated capability, giving rise to an effective enhancement of photodetection performance via the piezo-phototronic effect.