Ultralong room-temperature phosphorescence (RTP) materials showing persistent luminescence have attracted much attention in the fields of information encryption, light-emitting diodes (LEDs), sensors, data storage, bioimaging, and so on. As a large subset of ultralong RTP species, metal–organic halides (MOHs) have gained considerable attention recently due to their facilely tunable structures, controllable heavy atom effect, and strong quantum confinement effect. To date, challenges remain in deep understanding of the design methods and luminescence mechanism of MOHs with different dimensions. In this review, we have systematically summarized the recent developments in MOH materials from the perspective of self-assembled modes, including the ionic types from 2D to 0D MOHs and the molecular types from infinite to discrete structures. Then, design strategies for each kind of MOH are described. Finally, we introduce their potential applications including information encryption and photonic communication. Therefore, this review not only illustrates new RTP systems based on MOHs, but also presents their current issues and future trends, which could promote the research on MOHs for novel optical and photofunctional applications.
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