Stimuliâresponsive materials, showing bistable behaviors between two distinct states under external stimuli, can be potentially applied as basic components of modern electrical and electronic devices. 2D hybrid perovskites hold a promise to switch and tune dielectric bistability based on their solidâstate phase transitions. Here, strong dielectric enhancements are successfully actualized by virtue of light illumination in a DionâJacobson (DJ) type 2D hybrid perovskite, (HDA)(MA)2Pb3Br10 (1, where HDA is 1,6âhexanediammonium and MA is methylammonium). Upon heating, 1 exhibits an orderedâdisordered phase transition â 324 K (Tc), accompanying a transition from its low to high dielectric state. Strikingly, its lightâinduced dielectric constant changes are greatly enhanced with a magnitude up to 250% near the Tc, superior to most traditional inorganic phase transition materials. This process closely relates to the photoexcited dielectric effect that is caused by the interband photoâexcitation. Benefitting from the stability of DJâtype perovskite structure, the switching cycles of dielectric enhancement display operational stability with superior antiâfatigue characteristics. As per the knowledge, the findings of this strong dielectric enhancement are unprecedented in the family of 2D DJâtype hybrid perovskites, which will facilitate broad interest in exploiting new stimuliâresponsive materials to assemble highâperformance smart electronic devices.