A novel 1-［（phenylamino）-（phenylimine）］methylbenzimidazole［C20H16N4］was synthesized with N,N′-diphenylthiourea and benzimidazole as the starting material and neodymium nitrate hexahydrate as catalyst.The title compound was characterized by X-ray single-crystal diffraction,IR and elemental analysis.The crystal structure of the compound belongs to monoclinic system with space group P21/c.The cell parameters were as follows: a=0.921 6（10） nm,b=1.021 2（11） nm,c=1.879 6（17） nm,β=111.877（8）°,V=1.659（3） nm3,Z=4,Dc=1.251 g?cm3,F（000）=656,μ（Mo Kα）=0.077 mm-1,R=0.050 5 and ωR=0.130 1.The ionic recognition ability and thermal stability of the compound were investigated.