We present the synthesis of a lanthanoid-organic framework (LOF) featuring a dynamic structure that exhibits tunable magnetic properties. The LOF undergoes breathing and gate-opening phenomena in response to changes in DMF content and N2 sorption, leading to the emergence of new crystal phases with distinct characteristics. Notably, the desolvated form of the LOF excels as a single-ion magnet, while the fully activated structure demonstrates impressive qubit properties, exhibiting Rabi oscillations up to 60 K. Our work enables precise control over the LOF's geometry, allowing us to selectively tailor its magnetic behavior to achieve either of these two intriguing functionalities.
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