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Stimuli-responsive inorganic–organic frameworks (IOFs) are a class of functional materials, can controllably respond to one or more external stimuli. Among various organic linkers employed in IOF design, naphthalene diimides (NDIs) are of great interest because of their rigid and planar structure, electron-deficient character, and tunable electronic properties. The NDI derivatives are suitable for applications in optoelectronics, photochromic displays, electrochromic devices, chemical sensing, and rewritable media. In spite of the progress made recently in the synthesis of NDI-based ligands, NDI derivatives remain underexplored in crystalline hybrid materials (CHNs) due to synthetic challenges. This review comprehensively summarizes advances in NDI-CHNs, with a focus on highlighting structure–function relationships, as well as emerging functionalities, thereby offering theoretical insight and practical guidance for future research. • The research progress on crystalline hybrid materials (CHNs) based on NDI is systematically reviewed. • The structure and applications of NDI-CHNs are thoroughly summarized and analyzed. • The functions and mechanisms of NDI-CHNs in the field of stimulus response are discussed. • The transformative prospects of NDI-CHNs in intelligent health systems and environmental sustainability is envisioned. • The current synthetic challenges and limitations in the development of NDI-CHNs are identified.
You et al. (2026) studied this question.