An electrically modulated single‐/dual‐color imaging photodetector with fast response speed is developed based on a small molecule (COi8DFIC)/perovskite (CH3NH3PbBr3) hybrid film. Owing to the type‐I heterojunction, the device can facilely transform dual‐color images to single‐color images by applying a small bias voltage. The photodetector exhibits two distinct cut‐off wavelengths at ≈544 nm (visible region) and ≈920 nm (near‐infrared region), respectively, without any power supply. Its two peak responsivities are 0.16 A W−1 at ≈525 nm and 0.041 A W−1 at ≈860 nm with a fast response speed (≈102 ns). Under 0.6 V bias, the photodetector can operate in a single‐color mode with a peak responsivity of 0.09 A W−1 at ≈475 nm, showing a fast response speed (≈102 ns). A physical model based on band energy theory is developed to illustrate the origin of the tunable single‐/dual‐color photodetection. This work will stimulate new approaches for developing solution‐processed multifunctional photodetectors for imaging photodetection in complex circumstances.

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Three acceptor–acceptor (A–A) type conjugated polymers based on isoindigo and naphthalene diimide/perylene diimide are designed and synthesized to study the effects of building blocks and alkyl chains on the polymer properties and performance of all‐polymer photoresponse devices. Variation of the building blocks and alkyl chains can influence the thermal, optical, and electrochemical properties of the polymers, as indicated by thermogravimetric analysis, differential scanning calorimetry, UV–vis, cyclic voltammetry, and density functional theory calculations. Based on the A–A type conjugated polymers, the most efficient all‐polymer photovoltaic cells are achieved with an efficiency of 2.68%, and the first all‐polymer photodetectors are constructed with high responsivity (0.12 A W−1) and detectivity (1.2 × 1012 Jones), comparable to those of the best fullerene based organic photodetectors and inorganic photodetectors. Photoluminescence spectra, charge transport properties, and morphology of blend films are investigated to elucidate the influence of polymeric structures on device performances. This contribution demonstrates a strategy of systematically tuning the polymeric structures to achieve high performance all‐polymer photoresponse devices.