The high spin iron(II) chelate complex Fe1x2MeOH as well as its 1: 1 derivative with TCNE have been investigated with respect to cooperative magnetic properties. Fe1x2MeOH represents a magnetic chain compound, wherein an intermolecular interaction via hydrogen bonds between the OH-groups of axially coordinated methanol and the ester groups located on the ligand periphery is observed. The weak spontaneous magnetization below approximately 10 K indicates cooperative magnetic behavior. The reaction of the iron(II) chelate complex with the electron acceptor TCNE leads to a 1: 1 charge-transfer complex. The spontaneous magnetization occurs here below 10 K and is significantly higher compared to the magnetic iron(II) chelate chain compound.