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99Na0.01S, respectively.Organic ultralong room-temperature phosphorescence (OURTP) with a long-lived triplet excited state up to several seconds has triggered widespread research interests, but most OURTP materials are excited by only ultraviolet (UV) or blue light owing to their unique stabilized triplet- and solid-state emission feature. Here, we demonstrate that near-infrared- (NIR-) excitable OURTP molecules can be rationally designed by implanting intra/intermolecular charge transfer (CT) characteristics into H-aggregation to stimulate the effi