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Dissolution of LiCl or LiPF6 in pyridine or vinylpyridine and slow vapor diffusion of this solution with diethyl ether gives solvates of the lithium salts coordinated by pyridine ligands. In the case of the hexafluorophosphate salts, the chemical species formed are similar, namely binary salts with hexafluorophosphate counter-ions. In contrast, the solvates with LiCl are structurally dissimilar, with one forming a one-dimensional ionic polymer of fused LiCl rhombs and the other crystallizing as an isolated molecular unit with a complex array of van der Waals interactions of neighboring molecules.