Cyanide-bridged Mn(III)–Fe(III) complexes have been synthesized in order to find new molecular materials with interesting magnetic properties. 1D complexes of trans-dicyanoferrite(III), [Mn(5-Cl-salen)Fe(bpClb)(CN)2]·0.67MeCN·0.5H2O (1), [Mn(5-Cl-salen)Fe(bpb)(CN)2]·0.5H2O·MeOH (2), [Mn(5-Br-salen)Fe(bpb)(CN)2]·0.5H2O·MeOH (3), and [Mn(5-Me-salen)Fe(bpb)(CN)2]·0.5H2O·MeOH (4) have been prepared and characterized by X-ray single-crystal structure analysis and magnetic measurements. All complexes possesses 1D chains of alternate [Mn(5-R-salen)]+ and [Fe(bpRb)(CN)2]− units that are linked by two trans-cyanide ligands of [Fe(bpRb)(CN)2]−. Magnetic studies reveal that they exhibit overall intermetallic ferromagnetic coupling, while complex 4 shows a frequency-dependent AC magnetic susceptibility typical of a single-chain magnet.