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Foremost, practical applications of spin‐crossover (SCO) materials require control of the nature of the spin‐state coupling. In existing SCO materials, there is a single, well‐defined dimensionality relevant to the switching behavior. A new material, consisting of 1,2,4‐triazole‐based trimers coordinated into 1D chains by [Au(CN)2]− and spaced by anions and exchangeable guests, underwent SCO defined...