Molecular self-assembly is the spontaneous association of simple molecules into larger and ordered structures. 1 It is the basis of several natural processes, such as the formation of colloids, crystals, the generation of proteins, viruses and double helical DNA. 2 Molecular selfassembly has inspired strategies for the rational design of materials with specific chemical/physical properties, 3 becoming perhaps one of the most fascinating and important concepts in supramolecular chemistry. Here we report on a simple hydrochloride salt of fampridine which crystallises as four different structures, two of which adopt unusual selfassemblies consisting of polyhedral clusters of chloride and pyridinium ions. These two

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