A cyano-bridged bimetallic assembly, [Mn-III(salen)](2)[Fe-II(CN)(5)NO]center dot 2H(2)O [salen = N,N'-1,2-ethylenebis(salicylideneiminato)dianion], has been prepared and characterized structurally and magnetically. It crystallizes in the tetragonal space group P4/ncc with a = b = 14.813(2) , c = 17.093(5) , V = 3750.6(13) (3), Z = 4. In this complex, each [Fe(CN)(5)NO](2-) unit connects four [Mn(salen)](+) units with its four co-planar cyanide groups, and each [Mn(salen)](+) unit is linked to two [Fe(CN)(5)NO](2-) ions in trans-form, which results in a two-dimensional (2-D) network consisting of pillow-like octanuclear [-Fe-II-CN-Mn-III-NC-](4) units with dimensions: Fe-C = 1.943(3) , Ca parts per thousand N- = 1.139(4) , Mn-N = 2.326(3) , Fe-Ca parts per thousand N = 178.0(3)A degrees, Mn-Na parts per thousand C = 161.7(3)A degrees. The NO group of [Fe(CN)(5)NO](2-) remains monodentate and the bond angle of Fe-N-O is linear (180.0A degrees). The variable temperature magnetic susceptibilities, measured in the 1.8-300 K range, show a weak Mn-III center dot center dot center dot Mn-III antiferromagnetic interaction through the diamagnetic -NC-Fe-II-CN- bridges.