[Gd(DMF)(2)(H2O)(3)Cr(CN)(6)].H2O is the first lanthanide-transition metal
array with a flat two-dimensional brick-wall-like molecular structure. The
antiferromagnetic coupling between the adjacent Gd-Cr ions leads to intrala
yer ferrimagnetic correlation due to the noncancellation of spins. The long
-range magnetic ordering (T-N = 3.5 K) was observed for the first time in l
ow-dimensional cyano-bridged 4f-3d coordination polymers. Metamagnetic beha
vior was observed at 1.8 K arising from antiferromagnetic coupling between
the ferrimagnetic layers.