The synthesis, characterisation and magnetic properties of two series of po
lynuclear cyanide-bridged high spin molecules are presented. Tetranuclear c
ompounds of general formula (NC)(3)M(CNM'L-5)(3). 7H(2)O (M=Fe-III, Cr-III
and M' =Mn-III, Fe-III) are obtained by using peripheral complexes with pen
tadentate ligands. Pentanuclear complexes ((NC)(3)Cr[CNNi(ligand)(2)NC](3)C
r(CN)(3). 6H(2)O) are designed owing to steric hindrance induced by bulky b
identate ligands chelating the peripheral Ni-II complexes. The magnetic pro
perties show that ground states with spin up to 9 may be obtained.