optical modulation over large areas, these changes are potentially suitable for applications such as real-time holograms, [ 6 ] light-beam modulation for continuouswave lasers, and security media.Another possible approach to achieve large optical modulations under weak incoherent photoexcitation is through the accumulation of triplet excitons in materials, which can infl uence various physical properties such as absorption, [ 10 ] refractive index, [ 11 ] and magnetic properties. [ 12 ] Unlike the short lifetime of singlet excitons, [ 13 ] the lifetime of triplet excitons is long because the transition from the lowest triplet excited state (T 1 ) to the ground state (S 0 ) is intrinsically forbidden. [ 14 ] However, the accumulation of triplet excitons has been accomplished only by irradiation with strongly amplifi ed light pulses, such as neodymium-yttriumaluminum-garnet lasers and strong fl ash lamps. [ 15 ] This is because the lifetime of triplet excitons in organic compounds is generally shorter than a millisecond at room temperature (RT) in the presence of oxygen, as they are typically deactivated by molecular motion [ 16 ] and oxygen quenching. [ 17 ] We recently discovered that various aromatic carbon materials doped in amorphous hydroxyl steroidal compounds show T 1 lifetimes longer than 1 s at RT in air because of the rigidity and high oxygen barrier of the hydroxyl steroidal host. [ 18 ] In addition, optical limiting devices that operate under weak continuous incoherent photoexcitation in the presence of oxygen through the accumulation of long-lived RT triplet excitons have been demonstrated. [ 19 ] Therefore, it is anticipated that the triplet excitons of guests can be effectively accumulated in transparent amorphous fi lms of certain host-guest materials under weak continuous incoherent excitation light to trigger a large photoresponsive transmittance change of the fi lms.Here, we demonstrate photoresponsive neutral density fi lters for the whole range of visible light using the accumulation of long-lived RT triplet excitons under weak continuous photoexcitation. Transparent host-guest fi lms composed of a secondary amino-substituted deuterated aromatic carbon material as a guest and β-estradiol as an amorphous hydroxy steroidal host are prepared as photoresponsive optical fi lters. The guest shows no ground-state absorption but effi cient broad triplet-triplet (T-T) absorption of visible light, which is caused by the moderate charge transfer (CT) characteristics of the T-T absorption. In addition, the RT triplet lifetime ( τ ) of the guest in the host Excited-state absorption of materials is caused by instantaneous accumulation of excitons when irradiated with a high-intensity laser pulse. If excitons can be accumulated by irradiation with weak continuous incoherent light at room temperature (RT) in air, then excited-state absorption can be obtained over a large area, which is potentially useful for a variety of optical applications. Here, photoresponsive transmittance control using long-lived...