Three systems [Fe(III)(sal 2 -trien)](TCNQ) n ·X (n = 1, 2, X = MeOH, CH 3 CN, H 2 O) showing spin-crossover transition, conductivity and ferromagnetic coupling were synthesized and studied by X-ray diffraction, Montgomery method for resistivity, SQUID magnetometry and X-band EPR. Spin-spin interactions between local magnetic moments of Fe(III) ions and electron spins of organic TCNQ network were discovered and discussed within the framework of intermolecular superexchange coupling.