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Using the concept of isomorphous replacement applied to entire ligands, a C₃-symmetric trisulfonate ligand was substituted with a C₃-symmetric tris(hydrogen phosphonate) ligand in a proton conducting metal–organic framework (MOF). The resulting material, PCMOF2¹/₂, has its proton conduction raised 1.5 orders of magnitude compared to the parent material, to 2.1 × 10^–2 S cm^–1 at 90% relative humidity and 85 °C, while maintaining the parent MOF structure.