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Low-bandgap (E_g~1.25 eV) mixed tin-lead (Sn-Pb) perovskites are promising candidates for efficient solar cells and self-powered photodetectors; however, they suffer from huge amounts of defects due to the unintentional p-type self-doping. In this work, the synergistic effects of maltol and phenyl-C61-butyric acid methyl ester (PCBM) were achieved to improve the performance of low-bandgap perovskite solar cells (PSCs) and unbiased perovskite photodetectors (PPDs) by passivating the defects and tuning charge transfer dynamics. Maltol eliminated the Sn-related traps in perovskite films through a strong metal chelating effect, whereas PCBM elevated the built-in electric potential and thus improved voltage through the spike energy alignment. Combining both advantages of maltol and PCBM, high-quality perovskite films were obtained, enabling low-bandgap PSCs with the best efficiency of 20.62%. Moreover, the optimized PSCs were further applied as self-powered PPDs in a visible light communication system with a response time of 0.736 μs, presenting a satisfactory audio transmission capability.