Metal-organic frameworks (MOFs) represent one of the most diverse structural classes among solid state materials, yet few of them exhibit aperiodicity, or the existence of long-range order in the absence of translational symmetry. From this apparent conflict, a paradox has emerged: even though aperiodicity frequently arises in materials that contain the same bonding motifs as MOFs, aperiodic structures and MOFs appear to be nearly disjoint classes. In this perspective, we highlight a subset of the known aperiodic coordination polymers, including both incommensurate and quasicrystalline structures. We further comment upon possible reasons for the absence of such structures and propose routes to potentially access aperiodic MOFs.
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