ABSTRACT Integrating solar‐driven photovoltaics (PVs) with photo‐electrocatalytic (PEC) antibacterial systems presents a sustainable and efficient technology that operates entirely on renewable energy. Herein, we report a high‐performance, self‐powered PV‐PEC system enabled by wide‐bandgap (WBG) perovskite solar cells/modules (PSCs/PSMs). Specifically, 3‐Fluoro‐L‐Phenylalanine (3‐FLPA) is introduced as a molecular bridge in the n‐i‐p based perovskite devices. The carboxyl groups (–COOH) in 3‐FLP