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The chain-polymer Cu(II) breathing crystals C21H19CuF12N4O6 were studiedusing the x-ray diffraction and ab initio band structure calculations. We showthat the crystal structure modification at T=146 K, associated with the spincrossover transition, induces the changes of the orbital order in half of theCu sites. This in turn results in the switch of the magnetic interaction signin accordance with the Goodenough-Kanamori-Andersen theory of the couplingbetween the orbital and spin degrees of freedom.

Interplay between lattice, orbital, and magnetic degrees of freedom in the chain-polymer Cu(II) breathing crystals