Light-responsive spirotype compounds have been receiving attention as attractive smart materials because of their various potential applications in organic optoelectronic devices, based on organic field-effect transistors (OFETs). However, it still remains a challenge to apply the organic flash memory devices using spirotype compounds due to the relatively poor development of new photosensitive electret materials.Here, we report the synthesis of a novel photosensitive polymer electret material, spiropyran, containing poly(3,5-benzoic acid hexafluoroisopropylidene diphthalimide) (6FDA-DBA-SP), and the development of light-responsive flexible memory devices using the 6FDA-DBA-SP electret layer. The charge trapping properties of 6FDA-DBA-SP under light illumination were enhanced by the electron withdrawing properties and lowering energetic barrier of charge trapping between 6FDA-DBA-SP and pentacene analysed by measuring the electronic structures at the pentacene/6FDA-DBA-SP interfaces. The resulting OFETs showed enlarged hysteresis under white-light illumination and exhibited bi-stable current states after the light-assisted programing and erasing processes, and they were utilized in non-volatile flexible memory device applications. † Electronic supplementary information (ESI) available: Synthetic methods and analysis of 6FDA-DBA-SP; the 1 H-NMR spectrum, DSC curves, and TGA curves of 6FDA-DBA and 6FDA-DBA-SP; UV-Vis absorption spectra of SP-OH, 6FDA-DBA, and 6FDA-DBA-SP; electrical characteristics table of the SP-OFETs; transfer characteristics in the saturation regime of the SP-OFETs; transfer characteristics of the SP-OFETs during successive sweeps under different conditions (10 sweeps under dark conditions and 1 sweep under white-light); transfer characteristics of SP-OFETs as a function of applied bias time or voltage under dark conditions; transfer characteristics of SP-OFETs as a function of applied bias time under white-light illumination (sweeping from À40 V to 40 V); transfer characteristics of pentacene OFETs based on a polystyrene layer; comparative UPS spectra of pentacene and 6FDA-DBA-SP films in the dark or under white-light; (ahn) 2 versus hn plot of 6FDA-DBA-SP and pentacene films; current response to one-cycle switching behavior of SP-OFET memory devices; and transfer characteristics of the flexible SP-OFETs before and after bending in the dark. See