New bidimensional cyanido-bridged heterometallic coordination polymers, [{Co(L1)}3{Fe(CN)6}2]*6CH3OH*6H2O (1) and [{Fe(L2)}3{Co(CN)6}2]*2CH3OH*13H2O (2), have been assembled following a building-block approach (L1 and L2 are macrocyclic ligands obtained by the template condensation between 2,6-diacetylpyridine and 3,4-dioxaoctane-1,8-diamine, and triethylenetetramine, respectively). The crystal structure of 1 consists of honeycomb layers, each [FeIII(CN)6]3− unit connecting three [Co(L1)]2+ nodes through three facial cyanido groups. On the other hand, the self-assembly process between [CoIII(CN)6]3− and [Fe(L2)]2+ ions affords 2-D layers with a brick wall topology. Each [CoIII(CN)6]3− metalloligand is surrounded by three [Fe(L2)]2+ units, which adopt a meridional configuration around the cobalt metalloligand for compound 2. The magnetic properties of the two compounds have been investigated. Compound 1 shows a ferromagnetic order below 3 K. The magnetic properties of 2 are characteristic of non-interacting high spin FeII ions, which exhibit a moderate uniaxial magnetic anisotropy (D/kB = −5.5 K).