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Exploiting 2-(alkylsulfonyl)pyridines as 1,3-N,S-ligands, 1D CuI-based coordination polymers bearing unprecedented (CuI)n chains and possessing remarkable photophysical properties were constructed. Metallophilic interactions Cu鈰疌u in these compounds were studied theoretically by DFT calculations and topological analysis of electron density distribution. At room temperature, these coordination polymers show efficient thermally activated delayed fluorescence, phosphorescence or dual emission in the deep-blue to red range with outstandingly short decay times of 0.4–2.0 μs and good quantum performance. Moreover, the designed compounds emit strong X-ray radioluminescence with the quantum efficiency of up to an impressive 55% relative to well known all-inorganic bismuth germanate (BGO) scintillators. The presented findings push the boundaries in designing thermally activated delayed fluorescence and triplet emitters with very short decay times.