A new manganese(III) complex [Mn(L)(NCS)] (1) is synthesized from the Schiff base ligand N,N!-O-phenylenebis(4-methoxysalicylideneimine) (H2L: derived from the condensation of 4-methoxy salicylaldehyde with O-phenylene-diamine) with Mn(NO3)2!4H2O and KSCN in a methanol/water solvent mixture. This complex is characterized by elemental analysis, FT-IR and single crystal X-ray diffraction. It crystallizes in a monoclinic system, with space group P21/c and four molecules in the unit cell (Z = 4). The crystal structure shows [Mn(L)(NCS)] units joined together by the MnᄷS secondary bonding interaction (SBI) to form infinite zigzag chain structures.