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Tailored organoporous materials—the organic counterparts to inorganic nanoporous materials–have been prepared by a design strategy based on the observation that guanidinium organosulfonates (C(NH2)3RSO3) crystallize predictably in layered structures. The extension to disulfonates is shown to produce, among others, the motif shown in the Figure (the ovals are organodisulfonate pillars and the rectangles, guests).