Molecular crystals with guest-adaptable crystalline structures and properties are comparatively rare owing to their inherent reduced structural stability and malleability to support molecular variation. To overcome this intrinsic challenge, here we introduce structural stabilizing supramolecular interactions into a dinuclear material and henceforth demonstrate a dynamic structural and spin crossover property interchange between solvated (A center dot 3MeOH) and desolvated (A center dot O) products (A = [Fe-2II(oNTrz)(5)(NCS)(4)]; 4-(o-nitrobenzyl)imino-1,2,4-triazole). Relatively uncommon for molecular species, the guest molecules in A center dot 3MeOH are evolved (A center dot O) via a single-crystal to single-crystal transformation with affiliated phase transition resulting in a reversible transformation from one- to two-step spin crossover (SCO) transition character. We additionally present the water-saturated product (A center dot 3H(2)O), which distinctly shows an abrupt one-step SCO character with a 22 K wide thermal hysteresis loop. Detailed structure-property analysis highlights that the substantial structural malleability and guest-adaptable SCO properties of this dinuclear species are afforded by the supportive, yet flexible,supramolecular interaction pathways derived from the ligand functionalization.