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Inorganic semiconductor materials are best known for their superior physical properties, as well as their structural rigidity and stability. However, the poor solubility and solution-processability of these covalently bonded network structures has long been a serious drawback that limits their use in many important applications. Here, we present a unique and general approach to synthesize robust, solution-processable, and highly luminescent hybrid materials built on periodic and infinite inorganic modules. Structure analysis confirms that all compounds are composed of one-dimensional anionic chains of copper iodide (Cu_mI_m+2^2–) coordinated to cationic organic ligands via Cu–N bonds. The choice of ligands plays an important role in the coordination mode (μ¹-MC or μ²-DC) and Cu–N bond strength. Greatly suppressed nonradiative decay is achieved for the μ²-DC structures. Record high quantum yields of 85% (λ …