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The power conversion efficiency (PCE) of Cs2AgBiBr6-based perovskite solar cells (PSCs) is still low owing to the inherent defects of Cs2AgBiBr6 films. Herein, we demonstrate a carboxy-chlorophyll derivative (C-Chl)-sensitized mesoporous TiO2 (m-TiO2) film as an electron transport layer (ETL) to enhance and extend the absorption spectrum of Cs2AgBiBr6-based PSCs. The C-Chl-based device achieves a significantly improved PCE, exceeding 3% for the first time, with an increase of 27% in short-circuit current density. Optoelectronic investi