Abstract The quest for novel deformable image sensors with outstanding optoelectronic properties and large‐scale integration becomes a great impetus to exploit more advanced flexible photodetector (PD) arrays. Here, 10 × 10 flexible PD arrays with a resolution of 63.5 dpi are demonstrated based on as‐prepared perovskite arrays for photosensing and imaging. Large‐scale growth controllable CH 3 NH 3 PbI 3− x Cl x arrays are synthesized on a poly(ethylene terephthalate) substrate by using a two‐step sequential deposition method with the developed Al 2 O 3 ‐assisted hydrophilic–hydrophobic surface treatment process. The flexible PD arrays with high detectivity (9.4 × 10 11 Jones), large on/off current ratio (up to 1.2 × 10 3 ), and broad spectral response exhibit excellent electrical stability under large bending angle (θ = 150°) and superior folding endurance after hundreds of bending cycles. In addition, the device can execute the functions of capturing a real‐time light trajectory and detecting a multipoint light distribution, indicating that it has widespread potential in photosensing and imaging for optical communication, digital display, and artificial electronic skin applications.
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