Based on a synthetic strategy, extended anionic, homo- and bimetallic
oxalato-bridged transition-metal compounds with two- (2D) and three-di
mensional (3D) connectivities can be synthesized and crystallized. The
reby, the choice of the templating counterions will determine the crys
tal chemistry. Since the oxalato bridge is a mediator for both antifer
ro- and ferromagnetic interactions between similar and dissimilar meta
l ions, long-range magnetic ordering will occur. Examples of the deter
mination of magnetic structures in 2D and 3D compounds by means of ela
stic neutron scattering methods will be discussed. In addition, due to
the possibility of the variation of different metal ions in varying o
xidation states, interesting photophysical processes can be observed w
ithin the extended three-dimensional host/guest systems.